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Current strategies seek to overcome this limitation by enabling PEG shedding in response to pathological biochemical cues, but their dependence on heterogeneous microenvironments limits predictability and cross-route applicability. Here, we report a thermoresponsive PEG shedding strategy based on PEG\u2013lipid conjugates with oxanorbornadiene linkers that cleave at physiological temperature. By varying the linker structure, PEG shedding kinetics can be modulated over pharmacologically relevant time scales, enabling mRNA-lipid nanoparticles to undergo surface transitions from sterically shielded to cell-interactive states. In inhaled delivery, rapid PEG shedding after mucus traversal restored cellular uptake and markedly enhanced pulmonary mRNA expression, resulting in inhibition of pulmonary metastases. In systemic administration, intermediate PEG shedding preserved the circulation benefit of dense PEGylation while enabling subsequent intracellular delivery, leading to improved tumor expression and antitumor efficacy. These results establish kinetic programming of PEG shedding as a design principle for dynamically regulating nanoparticle biointerfaces across distinct delivery routes.<\/jats:p>","DOI":"10.1021\/jacs.6c09907","type":"journal-article","created":{"date-parts":[[2026,8,13]],"date-time":"2026-08-13T12:02:19Z","timestamp":1786622539000},"page":"36006-36021","source":"Crossref","is-referenced-by-count":0,"title":["Kinetically Programmed\nThermoresponsive Polyethylene\nGlycol Shedding from Lipid Nanoparticles Improves mRNA Delivery"],"prefix":"10.1021","volume":"148","author":[{"given":"Simin","family":"Sun","sequence":"first","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chen","family":"Yang","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]},{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yixing","family":"Wen","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haowei","family":"Zu","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haoyu","family":"Lu","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xingdi","family":"Cheng","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Juanjuan","family":"Han","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Han","family":"Ma","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuzhou","family":"Zhang","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yichen","family":"Jiang","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shiwei","family":"Mi","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1069-7265","authenticated-orcid":true,"given":"Xueguang","family":"Lu","sequence":"additional","affiliation":[{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]},{"name":"Institute of Chemistry, Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,13]]},"reference":[{"key":"2026090104500477300_cit1","doi-asserted-by":"publisher","first-page":"28","DOI":"10.1016\/j.addr.2015.09.012","article-title":"PEGylation as a\nStrategy for Improving Nanoparticle-Based Drug and Gene Delivery","volume":"99","author":"Suk","year":"2016","journal-title":"Adv. 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Adv."},{"key":"2026090104500477300_cit46","doi-asserted-by":"publisher","first-page":"2139","DOI":"10.1021\/ja2084338","article-title":"Nanoparticle\nSize and Surface Chemistry Determine Serum Protein Adsorption and\nMacrophage Uptake","volume":"134","author":"Walkey","year":"2012","journal-title":"J. Am. Chem. Soc."},{"issue":"4","key":"2026090104500477300_cit47","doi-asserted-by":"publisher","first-page":"1438","DOI":"10.1021\/ja309812z","article-title":"Nanoparticle\nAdhesion to the Cell Membrane and Its\nEffect on Nanoparticle Uptake Efficiency","volume":"135","author":"Lesniak","year":"2013","journal-title":"J.\nAm. Chem. Soc."},{"key":"2026090104500477300_cit48","doi-asserted-by":"publisher","first-page":"1909","DOI":"10.1021\/nl900031y","article-title":"Mediating\nTumor Targeting Efficiency of Nanoparticles through Design","volume":"9","author":"Perrault","year":"2009","journal-title":"Nano Lett."},{"key":"2026090104500477300_cit49","doi-asserted-by":"publisher","first-page":"815","DOI":"10.1038\/nnano.2011.166","article-title":"Accumulation of Sub-100\nnm Polymeric Micelles in Poorly Permeable Tumours Depends on Size","volume":"6","author":"Cabral","year":"2011","journal-title":"Nat. Nanotechnol."},{"issue":"5","key":"2026090104500477300_cit50","doi-asserted-by":"publisher","first-page":"16014","DOI":"10.1038\/natrevmats.2016.14","article-title":"Analysis of Nanoparticle Delivery\nto Tumours","volume":"1","author":"Wilhelm","year":"2016","journal-title":"Nat. Rev. Mater."},{"key":"2026090104500477300_cit51","doi-asserted-by":"publisher","first-page":"9875","DOI":"10.1021\/acsnano.5c19757","article-title":"The Impact\nof Polyethylene Glycol Lipid Anchors on\nthe Physicochemical Properties, Protein Corona, Function, and Biodistribution\nof Lipid Nanoparticles","volume":"20","author":"Lu","year":"2026","journal-title":"ACS Nano"},{"issue":"1","key":"2026090104500477300_cit52","doi-asserted-by":"publisher","first-page":"8699.s","DOI":"10.1038\/s41467-025-63726-2","article-title":"Protein Corona Formed on Lipid Nanoparticles\nCompromises Delivery Efficiency of mRNA Cargo","volume":"16","author":"Voke","year":"2025","journal-title":"Nat. Commun."}],"container-title":["Journal of the American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c09907","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/33\/36006\/66522749\/jacs.6c09907.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/33\/36006\/66522749\/jacs.6c09907.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,1]],"date-time":"2026-09-01T08:50:14Z","timestamp":1788252614000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/33\/36006\/5254148\/Kinetically-Programmed-Thermoresponsive"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,13]]},"references-count":52,"journal-issue":{"issue":"33","published-online":{"date-parts":[[2026,8,13]]},"published-print":{"date-parts":[[2026,8,26]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c09907","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,13]]}}}