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Here, we delineate a pathogenic cascade wherein the impaired dephosphorylation of hyperphosphorylated tau (p-tau) leads to its aggregation, which is amplified by microglia-mediated propagation. To combat this p-tau cascade, we developed a glycoengineered proteolysis targeting chimera (PROTAC) nanoparticle for lesion-specific p-tau modulation therapy. We first synthesized a library of p-tau PROTACs and identified a lead compound (namely, PROTAC-7) that effectively degraded diverse p-tau species across multiple cellular and animal models of tauopathy. The glycoengineered nanoparticles were then prepared by coassembly of galactose\/cyclodextrin-grafted polysialic acid with a microglial scavenger PLX and a reactive oxygen species (ROS)-sensitive heterodimer of PROTAC-7 and memantine (an activator of protein phosphatase 2A). Upon systemic administration, the glycoengineered PROTAC nanoparticles achieved brain-targeted delivery of the therapeutics via glycemic-gradient-mediated transport across the blood\u2013brain barrier. Upon activation in ROS-rich AD lesions, the nanoparticles released their payload for spatially confined p-tau degradation and suppression of tau phosphorylation and spread. This coordinated modulation strategy markedly reversed tau pathology, restored synaptic plasticity, and ameliorated cognitive deficits in multiple mouse models of AD.<\/jats:p>","DOI":"10.1021\/jacs.6c05275","type":"journal-article","created":{"date-parts":[[2026,6,4]],"date-time":"2026-06-04T19:15:57Z","timestamp":1780600557000},"page":"24287-24305","source":"Crossref","is-referenced-by-count":2,"title":["Glycoengineered\nHost-Guest Nanoparticles Potentiate\nAlzheimer\u2019s Disease Therapy via Lesion-Specific Modulation\nof Tau Pathology"],"prefix":"10.1021","volume":"148","author":[{"given":"Yi","family":"Lai","sequence":"first","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaxing","family":"Pan","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]},{"name":"Fudan University , , ,","place":["Shanghai, China, 200040"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuejiao","family":"Gu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-8150-7378","authenticated-orcid":true,"given":"Chuan","family":"Zhou","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenfang","family":"Yang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]},{"name":"Nanjing University of Chinese Medicine , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qian","family":"Zhao","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zifan","family":"Zhu","sequence":"additional","affiliation":[{"name":"East China Normal University , , ,","place":["Shanghai, China, 200241"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanhong","family":"Duan","sequence":"additional","affiliation":[{"name":"East China Normal University , , ,","place":["Shanghai, China, 200261"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Li","family":"Lei","sequence":"additional","affiliation":[{"name":"Guizhou Medical University , , ,","place":["Guiyang, China, 561113"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ying","family":"Fu","sequence":"additional","affiliation":[{"name":"University of Strathclyde , , ,","place":["Glasgow, U.K., G1 1RD"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2877-2040","authenticated-orcid":true,"given":"Haiyan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Boyan","family":"Fang","sequence":"additional","affiliation":[{"name":"Capital Medical University , , ,","place":["Beijing, China, 100070"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8996-4065","authenticated-orcid":true,"given":"Tianfeng","family":"Xu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4391-2507","authenticated-orcid":true,"given":"Zhiai","family":"Xu","sequence":"additional","affiliation":[{"name":"East China Normal University , , ,","place":["Shanghai, China, 200241"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3398-0880","authenticated-orcid":true,"given":"Haijun","family":"Yu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Shanghai, China, 201203"]},{"name":"Nanjing University of Chinese Medicine , , ,","place":["Nanjing, China, 210023"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,6,4]]},"reference":[{"issue":"4","key":"2026073023145904700_cit1","doi-asserted-by":"publisher","first-page":"693","DOI":"10.1016\/j.cell.2022.12.032","article-title":"Hallmarks\nof neurodegenerative diseases","volume":"186","author":"Wilson","year":"2023","journal-title":"Cell"},{"issue":"9","key":"2026073023145904700_cit2","doi-asserted-by":"publisher","first-page":"2187","DOI":"10.1038\/s41591-023-02505-2","article-title":"Emerging diagnostics\nand therapeutics for Alzheimer\ndisease","volume":"29","author":"Self","year":"2023","journal-title":"Nat. Med."},{"issue":"12","key":"2026073023145904700_cit3","doi-asserted-by":"publisher","first-page":"863","DOI":"10.1038\/nrd.2017.155","article-title":"Tau-based therapies\nin neurodegeneration: opportunities and challenges","volume":"16","author":"Li","year":"2017","journal-title":"Nat. Rev. Drug Discovery"},{"issue":"1","key":"2026073023145904700_cit4","doi-asserted-by":"publisher","first-page":"15","DOI":"10.1038\/nrneurol.2015.225","article-title":"Tau and neurodegenerative disease: the story so far","volume":"12","author":"Iqbal","year":"2016","journal-title":"Nat. Rev. Neurol."},{"issue":"2","key":"2026073023145904700_cit5","doi-asserted-by":"publisher","first-page":"312","DOI":"10.1016\/j.cell.2019.09.001","article-title":"Alzheimer Disease: An Update on Pathobiology\nand Treatment\nStrategies","volume":"179","author":"Long","year":"2019","journal-title":"Cell"},{"issue":"11","key":"2026073023145904700_cit6","doi-asserted-by":"publisher","first-page":"845","DOI":"10.1038\/s41580-024-00753-9","article-title":"Cellular and pathological\nfunctions of tau","volume":"25","author":"Parra Bravo","year":"2024","journal-title":"Nat. Rev. Mol. Cell Biol."},{"issue":"6","key":"2026073023145904700_cit7","doi-asserted-by":"publisher","first-page":"464","DOI":"10.1038\/nrd2111","article-title":"Untangling tau hyperphosphorylation\nin drug design\nfor neurodegenerative diseases","volume":"6","author":"Mazanetz","year":"2007","journal-title":"Nat. Rev. Drug\nDiscovery"},{"issue":"7","key":"2026073023145904700_cit8","doi-asserted-by":"publisher","first-page":"399","DOI":"10.1038\/s41582-018-0013-z","article-title":"Tau-targeting\ntherapies for Alzheimer disease","volume":"14","author":"Congdon","year":"2018","journal-title":"Nat. Rev. Neurol."},{"issue":"6532","key":"2026073023145904700_cit9","doi-asserted-by":"publisher","DOI":"10.1126\/science.abb8255","article-title":"Tau: Enabler\nof diverse brain disorders\nand target of rapidly evolving therapeutic strategies","volume":"371","author":"Chang","year":"2021","journal-title":"Science"},{"key":"2026073023145904700_cit10","doi-asserted-by":"publisher","first-page":"102594","DOI":"10.1016\/j.arr.2024.102594","article-title":"Unknown\nroles of tau pathology in neurological disorders. Challenges and new\nperspectives","volume":"103","author":"Olesen","year":"2025","journal-title":"Ageing Res. Rev."},{"issue":"12","key":"2026073023145904700_cit11","doi-asserted-by":"publisher","first-page":"715","DOI":"10.1038\/s41582-023-00883-2","article-title":"Tau-targeting\ntherapies for Alzheimer disease: current status and future directions","volume":"19","author":"Congdon","year":"2023","journal-title":"Nat. Rev. Neurol."},{"issue":"6","key":"2026073023145904700_cit12","doi-asserted-by":"publisher","first-page":"1437","DOI":"10.1038\/s41591-023-02326-3","article-title":"Tau-targeting\nantisense oligonucleotide MAPT(Rx) in mild Alzheimer\u2019s disease:\na phase 1b, randomized, placebo-controlled trial","volume":"29","author":"Mummery","year":"2023","journal-title":"Nat. Med."},{"issue":"9","key":"2026073023145904700_cit13","doi-asserted-by":"publisher","first-page":"591","DOI":"10.1038\/nrd.2016.176","article-title":"Pharma pumps\nup anti-tau Alzheimer pipeline despite first Phase III failure","volume":"15","author":"Mullard","year":"2016","journal-title":"Nat. Rev. Drug Discovery"},{"issue":"11","key":"2026073023145904700_cit14","doi-asserted-by":"publisher","first-page":"5279","DOI":"10.7150\/thno.55680","article-title":"A novel small-molecule\nPROTAC selectively promotes tau clearance to improve cognitive functions\nin Alzheimer-like models","volume":"11","author":"Wang","year":"2021","journal-title":"Theranostics"},{"issue":"5","key":"2026073023145904700_cit15","doi-asserted-by":"publisher","first-page":"3448","DOI":"10.1021\/acs.jmedchem.3c01719","article-title":"Discovery of Effective\nDual PROTAC Degraders for Neurodegenerative\nDisease-Associated Aggregates","volume":"67","author":"Zhu","year":"2024","journal-title":"J. Med. Chem."},{"issue":"1","key":"2026073023145904700_cit16","doi-asserted-by":"publisher","first-page":"41","DOI":"10.1186\/s13024-023-00630-7","article-title":"Targeted\ndegradation of \u03b1-synuclein\naggregates in Parkinson\u2019s disease using the AUTOTAC technology","volume":"18","author":"Lee","year":"2023","journal-title":"Mol. Neurodegener."},{"issue":"4","key":"2026073023145904700_cit17","doi-asserted-by":"publisher","first-page":"453","DOI":"10.1016\/j.chembiol.2016.02.016","article-title":"Specific Knockdown of Endogenous\nTau Protein by Peptide-Directed Ubiquitin-Proteasome Degradation","volume":"23","author":"Chu","year":"2016","journal-title":"Cell Chem. Biol."},{"issue":"1","key":"2026073023145904700_cit18","doi-asserted-by":"publisher","first-page":"904","DOI":"10.1038\/s41467-022-28520-4","article-title":"The AUTOTAC\nchemical biology platform for targeted protein degradation via the\nautophagy-lysosome system","volume":"13","author":"Ji","year":"2022","journal-title":"Nat. Commun."},{"issue":"3","key":"2026073023145904700_cit19","doi-asserted-by":"publisher","first-page":"654","DOI":"10.1021\/acsptsci.4c00733","article-title":"Targeting Tau Protein with Proximity\nInducing Modulators: A New Frontier to Combat Tauopathies","volume":"8","author":"Uliassi","year":"2025","journal-title":"ACS Pharmacol. Transl. Sci."},{"key":"2026073023145904700_cit20","doi-asserted-by":"publisher","DOI":"10.7554\/elife.45457","article-title":"Targeted degradation\nof aberrant tau in frontotemporal\ndementia patient-derived neuronal cell models","volume":"8","author":"Silva","year":"2019","journal-title":"eLife"},{"key":"2026073023145904700_cit21","doi-asserted-by":"publisher","first-page":"801179","DOI":"10.3389\/fncel.2022.801179","article-title":"Discovery and Optimization of Tau\nTargeted Protein\nDegraders Enabled by Patient Induced Pluripotent Stem Cells-Derived\nNeuronal Models of Tauopathy","volume":"16","author":"Silva","year":"2022","journal-title":"Front. Cell. Neurosci."},{"key":"2026073023145904700_cit22","doi-asserted-by":"publisher","DOI":"10.1038\/s41551-025-01525-2","article-title":"Targeted clearance\nof extracellular Tau using aptamer-armed\nmonocytes alleviates neuroinflammation in mice with Alzheimer\u2019s\ndisease","author":"Zhuo","year":"2025","journal-title":"Nat. Biomed. Eng."},{"issue":"1","key":"2026073023145904700_cit23","doi-asserted-by":"publisher","first-page":"217","DOI":"10.1038\/s41392-023-01481-w","article-title":"The blood-brain\nbarrier: structure, regulation, and drug delivery","volume":"8","author":"Wu","year":"2023","journal-title":"Signal Transduct. Target Ther."},{"issue":"2","key":"2026073023145904700_cit24","doi-asserted-by":"publisher","first-page":"215","DOI":"10.1016\/j.jalz.2017.08.012","article-title":"A systematic integrated\nanalysis of brain expression profiles reveals YAP1 and other prioritized\nhub genes as important upstream regulators in Alzheimer\u2019s disease","volume":"14","author":"Xu","year":"2018","journal-title":"Alzheimers Dement."},{"issue":"43","key":"2026073023145904700_cit25","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abg4980","article-title":"Microglia become hypofunctional and\nrelease metalloproteases and tau seeds when phagocytosing live neurons\nwith P301S tau aggregates","volume":"7","author":"Brelstaff","year":"2021","journal-title":"Sci. Adv."},{"issue":"1","key":"2026073023145904700_cit26","doi-asserted-by":"publisher","first-page":"1969","DOI":"10.1038\/s41467-022-29552-6","article-title":"Microglial NF-kappaB\ndrives tau spreading and toxicity in a mouse\nmodel of tauopathy","volume":"13","author":"Wang","year":"2022","journal-title":"Nat. Commun."},{"issue":"6656","key":"2026073023145904700_cit27","doi-asserted-by":"publisher","DOI":"10.1126\/science.add6696","article-title":"TRIM11 protects\nagainst tauopathies and is down-regulated in Alzheimer\u2019s disease","volume":"381","author":"Zhang","year":"2023","journal-title":"Science"},{"issue":"6","key":"2026073023145904700_cit28","doi-asserted-by":"publisher","first-page":"559","DOI":"10.1046\/j.1440-1711.1999.00870.x","article-title":"Carboxyfluorescein succinimidyl ester-based proliferative\nassays for assessment of T cell function in the diagnostic laboratory","volume":"77","author":"Fulcher","year":"1999","journal-title":"Immunol. Cell Bio."},{"key":"2026073023145904700_cit29","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202314132","article-title":"PROTAC Prodrug-Integrated\nNanosensitizer for Potentiating Radiation\nTherapy of Cancer","volume":"36","author":"Zhang","year":"2024","journal-title":"Adv. Mater."},{"issue":"10","key":"2026073023145904700_cit30","doi-asserted-by":"publisher","first-page":"4266","DOI":"10.1016\/j.apsb.2024.04.007","article-title":"Characteristic roadmap\nof linker governs the rational design of PROTACs","volume":"14","author":"Dong","year":"2024","journal-title":"Acta Pharm. Sin. B"},{"issue":"21","key":"2026073023145904700_cit31","doi-asserted-by":"publisher","first-page":"5967","DOI":"10.1016\/j.cell.2024.08.024","article-title":"Co-opting templated\naggregation to degrade pathogenic tau assemblies and improve motor\nfunction","volume":"187","author":"Miller","year":"2024","journal-title":"Cell"},{"issue":"17","key":"2026073023145904700_cit32","doi-asserted-by":"publisher","first-page":"15317","DOI":"10.1074\/jbc.M110.209296","article-title":"Seeding of normal\nTau by pathological Tau conformers\ndrives pathogenesis of Alzheimer-like tangles","volume":"286","author":"Guo","year":"2011","journal-title":"J. Biol. Chem."},{"issue":"6712","key":"2026073023145904700_cit33","doi-asserted-by":"publisher","first-page":"1009","DOI":"10.1126\/science.adp5186","article-title":"Aggregate-selective\nremoval of pathological tau by clustering-activated degraders","volume":"385","author":"Benn","year":"2024","journal-title":"Science"},{"issue":"12","key":"2026073023145904700_cit34","doi-asserted-by":"publisher","DOI":"10.1371\/journal.pone.0145441","article-title":"Memantine\nAttenuates Alzheimer\u2019s Disease-Like Pathology and Cognitive\nImpairment","volume":"10","author":"Wang","year":"2015","journal-title":"PLoS One"},{"issue":"7953","key":"2026073023145904700_cit35","doi-asserted-by":"publisher","first-page":"668","DOI":"10.1038\/s41586-023-05788-0","article-title":"Microglia-mediated\nT cell infiltration drives neurodegeneration in tauopathy","volume":"615","author":"Chen","year":"2023","journal-title":"Nature"},{"issue":"4","key":"2026073023145904700_cit36","doi-asserted-by":"publisher","first-page":"530","DOI":"10.1038\/s41593-018-0090-8","article-title":"Repopulated microglia are solely derived from the proliferation\nof\nresidual microglia after acute depletion","volume":"21","author":"Huang","year":"2018","journal-title":"Nat.\nNeurosci."},{"issue":"1","key":"2026073023145904700_cit37","doi-asserted-by":"publisher","first-page":"3758","DOI":"10.1038\/s41467-019-11674-z","article-title":"Sustained\nmicroglial depletion with CSF1R inhibitor\nimpairs parenchymal plaque development in an Alzheimer\u2019s disease\nmodel","volume":"10","author":"Spangenberg","year":"2019","journal-title":"Nat. Commun."},{"issue":"2","key":"2026073023145904700_cit38","doi-asserted-by":"publisher","first-page":"872","DOI":"10.1021\/acschemneuro.8b00402","article-title":"Targeting Neuroinflammation\nas a\nTherapeutic Strategy for Alzheimer\u2019s Disease: Mechanisms, Drug\nCandidates, and New Opportunities","volume":"10","author":"Fu","year":"2019","journal-title":"ACS Chem.\nNeurosci."},{"issue":"8","key":"2026073023145904700_cit39","doi-asserted-by":"publisher","first-page":"3340","DOI":"10.1021\/acschemneuro.9b00333","article-title":"Understanding\nthe Role of Systemic\nInflammation in Alzheimer\u2019s Disease","volume":"10","author":"Walker","year":"2019","journal-title":"ACS Chem. Neurosci."},{"issue":"1","key":"2026073023145904700_cit40","doi-asserted-by":"publisher","first-page":"1001","DOI":"10.1038\/s41467-017-00952-3","article-title":"Glycaemic control boosts glucosylated\nnanocarrier crossing the BBB into the brain","volume":"8","author":"Anraku","year":"2017","journal-title":"Nat. Commun."},{"issue":"21","key":"2026073023145904700_cit41","doi-asserted-by":"publisher","first-page":"8662","DOI":"10.1073\/pnas.1307152110","article-title":"Transcytosis and\nbrain uptake of transferrin-containing nanoparticles by tuning avidity\nto transferrin receptor","volume":"110","author":"Wiley","year":"2013","journal-title":"Proc. Natl. Acad. Sci.\nU.S.A."},{"issue":"5","key":"2026073023145904700_cit42","doi-asserted-by":"publisher","first-page":"667","DOI":"10.1007\/s00401-014-1254-6","article-title":"A novel in vivo model of tau propagation with rapid\nand progressive neurofibrillary tangle pathology: the pattern of spread\nis determined by connectivity, not proximity","volume":"127","author":"Ahmed","year":"2014","journal-title":"Acta Neuropathol."},{"issue":"1","key":"2026073023145904700_cit43","doi-asserted-by":"publisher","first-page":"71","DOI":"10.1186\/s13195-024-01439-2","article-title":"Glymphatic\ninhibition exacerbates tau propagation in an Alzheimer\u2019s disease\nmodel","volume":"16","author":"Lopes","year":"2024","journal-title":"Alzheimer Res. Ther."},{"issue":"37","key":"2026073023145904700_cit44","doi-asserted-by":"publisher","first-page":"16930","DOI":"10.1021\/jacs.2c05499","article-title":"Discovery of XL01126: A Potent, Fast, Cooperative,\nSelective, Orally Bioavailable, and Blood-Brain Barrier Penetrant\nPROTAC Degrader of Leucine-Rich Repeat Kinase 2","volume":"144","author":"Liu","year":"2022","journal-title":"J. Am. Chem. 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