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Drawing inspiration from this natural mechanism, we developed covalent organic frameworks (COFs) with programmable nanoscale confinement, achieved via topology\u2010directed assembly. This design enables precise spatiotemporal regulation of ROS generation and scavenging, thereby facilitating highly efficient and unprecedented dual\u2010potential electrochemiluminescence (ECL). The resulting confined COF architecture exhibits enhanced electronic coupling, attributable to dense \u03c0\u2010stacking, and a well\u2010ordered, continuous hydrogen\u2010bonding network templated by functionalized pore walls. By mimicking enzymatic proton\u2010coupled electron transfer (PCET), the confined environment not only promotes site\u2010specific ROS generation from electrocatalytic water oxidation but also directs ROS\u2010mediated redox consumption pathways toward selective population of emissive excited states. As a result, we report the first dual\u2010potential ECL emission in a COF\u2010based system, achieving cathodic and anodic ECL efficiencies of 40.5% and 21.2%, respectively, representing 11.3\u2010 and 8.2\u2010fold enhancements relative to analogous unconfined COFs. Moreover, size\u2010selective binding of UO\n                    <jats:sub>2<\/jats:sub>\n                    <jats:sup>2+<\/jats:sup>\n                    within the confined pores provides direct experimental evidence for confinement\u2010enabled ROS regulation, yielding quantitative, analyte\u2010responsive ECL signals. Collectively, these findings establish a broadly applicable principle of confinement\u2010directed reactivity, grounded in mechanistic understanding and offering a rational, structure\u2010function\u2010guided strategy for the design of advanced functional materials.\n                  <\/jats:p>","DOI":"10.1002\/anie.7934270","type":"journal-article","created":{"date-parts":[[2026,10,2]],"date-time":"2026-10-02T07:38:10Z","timestamp":1790926690000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Topology\u2010Directed Biomimetic Confinement in Covalent Organic Frameworks Couples Electrocatalytic Water Activation to Reactive Oxygen Species Evolution for Dual\u2010Potential Electrochemiluminescence"],"prefix":"10.1002","author":[{"given":"Qiao\u2010Qiao","family":"Jiang","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Nanchang University  Nanchang 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