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However, achieving efficient recruitment and activation of T cells while blocking immune suppression remains a critical challenge. Current strategies mainly focus on the blockade of the PD\u20101\/PD\u2010L1 axis, with limited attention to reprogramming immune functions on the tumor cell surface. Here, we report a \u201clocalized oxidation\u2010covalent assembly\u201d strategy that achieves precise modification of PD\u2010L1 on the cell surface through glycan oxidation, thereby harnessing bioorthogonal reactions to induce the in situ construction of artificial topological nanostructures (ATNs), which subsequently augment T cell\u2010mediated antitumor immunity. ATNs not only block the PD\u20101\/PD\u2010L1 axis to relieve immune suppression but also recruit and activate T cells through transmembrane bridging interactions, mimicking bispecific T cell engagers (BiTEs) and markedly enhancing antitumor immune responses. Mechanistic studies revealed that N\u2010glycosylation sites are critical for probe\u2010mediated aldehyde modification of PD\u2010L1. We further demonstrated that the ATNs achieve spatially precise T cell recruitment and activation via PD\u2010L1\u2010dependent localization, enabling programmable immune regulation. Overall, this approach not only underscores the potential of glycan oxidation\u2010driven self\u2010assembly in immune modulation but also provides a versatile chemical biology tool for the precise reprogramming of immune checkpoint functions.<\/jats:p>","DOI":"10.1002\/anie.5894316","type":"journal-article","created":{"date-parts":[[2026,7,3]],"date-time":"2026-07-03T17:30:02Z","timestamp":1783099802000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Covalently PD\u2010L1 Anchoring Drives Bispecific Nanostructure Assembly for Spatial Control of T Cell Recruitment and Activation"],"prefix":"10.1002","volume":"65","author":[{"given":"Fengzhen","family":"Zhang","sequence":"first","affiliation":[{"name":"Department Basic Medicine Research and Innovation Center for Novel Target and Therapeutic Intervention College of Pharmacy Ministry of Education Chongqing Medical University  Chongqing 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