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Metal\u2013phenolic networks (MPNs), as a class of novel hybrid materials, hold great promise for overcoming brain delivery bottlenecks and enabling precise synergistic therapy by leveraging their unique physicochemical properties. However, a comprehensive synthesis of MPN designs tailored specifically to the distinct pathological mechanisms underlying brain disorders is currently lacking. Methods: In this review, we systematically outline the foundational building blocks of MPNs and their diverse nanostructure engineering strategies. Building on this, we closely align MPN customization with the four core pathological pillars of brain diseases, thoroughly summarizing advanced design strategies and synergistic therapeutic mechanisms. Additionally, we prospectively discuss emerging innovative approaches, including the targeting of neutrophil extracellular traps (NETs) to modulate the immunosuppressive tumor microenvironment. Outlook: Finally, we critically examine the pivotal obstacles hindering the clinical translation of MPNs, particularly concerning uncertainties in long-term biosafety and in vivo metabolism, metal-specific neurotoxicity and coordination-stability-governed metal release kinetics, challenges in quality control during scalable production, and the unpredictable interference of the protein corona. Conclusions: In this review, we provide a robust theoretical foundation for the rational design of mechanism-driven MPNs, while offering forward-looking perspectives to accelerate their clinical translation from bench to bedside for the precise management of brain diseases.<\/jats:p>","DOI":"10.3390\/pharmaceutics18091192","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T10:25:43Z","timestamp":1789986343000},"page":"1192","update-policy":"https:\/\/doi.org\/10.3390\/mdpi_crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Mechanism-Driven Design of Metal\u2013Phenolic Networks: From Precision Assembly to Multidimensional Synergistic Therapy for Brain Diseases"],"prefix":"10.3390","volume":"18","author":[{"given":"Mengyue","family":"Ni","sequence":"first","affiliation":[{"name":"Department of Medicinal Chemistry, College of Pharmaceutical Sciences of Capital Medical University, Beijing 100069, China"},{"name":"Beijing Key Laboratory of Intelligent Clinical Data and AI-Driven Innovative Drug Development, Beijing Laboratory of Biomedical Materials, Laboratory for Clinical Medicine, Capital Medical University, Beijing 100069, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Hu","sequence":"additional","affiliation":[{"name":"Department of Medicinal Chemistry, College of Pharmaceutical Sciences of Capital Medical University, Beijing 100069, China"},{"name":"Beijing Key Laboratory of Intelligent Clinical Data and AI-Driven Innovative Drug Development, Beijing Laboratory of Biomedical Materials, Laboratory for Clinical Medicine, Capital Medical University, Beijing 100069, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8959-2596","authenticated-orcid":false,"given":"Di","family":"Zhu","sequence":"additional","affiliation":[{"name":"Department of Pharmacy, Xuanwu Hospital of Capital Medical University, Beijing 100053, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Boya","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Medicinal Chemistry, College of Pharmaceutical Sciences of Capital Medical University, Beijing 100069, China"},{"name":"Beijing Key Laboratory of Intelligent Clinical Data and AI-Driven Innovative Drug Development, Beijing Laboratory of Biomedical Materials, Laboratory for Clinical Medicine, Capital Medical University, Beijing 100069, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3588-5334","authenticated-orcid":false,"given":"Yijiang","family":"Jia","sequence":"additional","affiliation":[{"name":"Department of Medicinal Chemistry, College of Pharmaceutical Sciences of Capital Medical University, Beijing 100069, China"},{"name":"Beijing Key Laboratory of Intelligent Clinical Data and AI-Driven Innovative Drug Development, Beijing Laboratory of Biomedical Materials, Laboratory for Clinical Medicine, Capital Medical University, Beijing 100069, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Lu","sequence":"additional","affiliation":[{"name":"Department of Medicinal Chemistry, College of Pharmaceutical Sciences of Capital Medical University, Beijing 100069, China"},{"name":"Beijing Key Laboratory of Intelligent Clinical Data and AI-Driven Innovative Drug Development, Beijing Laboratory of Biomedical Materials, Laboratory for Clinical Medicine, Capital Medical University, Beijing 100069, China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3842-7627","authenticated-orcid":false,"given":"Yuji","family":"Wang","sequence":"additional","affiliation":[{"name":"Department of Medicinal Chemistry, College of Pharmaceutical Sciences of Capital Medical University, Beijing 100069, China"},{"name":"Beijing Key Laboratory of Intelligent Clinical Data and AI-Driven Innovative Drug Development, Beijing Laboratory of Biomedical Materials, Laboratory for Clinical Medicine, Capital Medical University, Beijing 100069, China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"1968","published-online":{"date-parts":[[2026,9,21]]},"reference":[{"key":"ref_1","doi-asserted-by":"crossref","first-page":"106808","DOI":"10.1016\/j.neubiorev.2026.106808","article-title":"Global prevalence and disability burden of brain disorders: Impact of neurological, mental, and substance use disorders","volume":"188","author":"Salehinejad","year":"2026","journal-title":"Neurosci. 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