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However, a tricky trade\u2010off remains between active\u2010site density and accessibility. Here we describe a trade\u2010off\u2010breaking design of sulfur\u2010modulated COF superstructures (TD\u2010COFS) via synergistic geometric\u2010electronic structure engineering. Flower\u2010shaped TD\u2010COFS is constructed by intermolecular H\u2010bonding and \u03c0\u2010\u03c0 stacking self\u2010assembly of tricarbonyl\u2010benzothiazole motifs, maximizing exposure of well\u2010organized multi\u2010protophilic active sites and \u03c0\u2010electron delocalization routes. Electron\u2010rich S\u2010heterocyclic benzothiazole (replacing N\u2010containing bipyridine, TM\u2010COFS) increases the electronegativity of TD\u2010COFS and reduces the redox barrier (S\u00a0&lt;\u00a0N), enabling synchronous optimization of molecular charge distribution and electronic bandgap (\u22120.75\/1.82 vs. \u22120.52\/2.47\u00a0eV of TM\u2010COFS). Furthermore, sulfur modulation boosts proton\u2010transfer redox activity with a low activation energy (0.23\u00a0eV), and achieves full accessibility of highly dense protophilic sites in TD\u2010COFS (99.3%\u00a0vs. 0.34\u00a0eV\/84.7% of TM\u2010COFS), liberating high capacity (356\u00a0mAh\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) and cycling stability (70\u00a0000 cycles). Besides, the assembled soft\u2010packed all\u2010organic proton batteries deliver state\u2010of\u2010the\u2010art capacity (161\u00a0mAh\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), energy density (81\u00a0Wh kg\n                    <jats:sup>\u22121<\/jats:sup>\n                    <jats:sub>cell<\/jats:sub>\n                    ), and life (3000 cycles). This work broadens the design philosophy of structured\u2010tailored COFs with highly dense and accessible protophilic sites for better proton batteries.\n                  <\/jats:p>","DOI":"10.1002\/anie.1065026","type":"journal-article","created":{"date-parts":[[2026,8,11]],"date-time":"2026-08-11T13:04:00Z","timestamp":1786453440000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Sulfur\u2010Modulated Covalent Organic Framework Superstructures With Highly Dense and Fully Accessible Protophilic Sites for High\u2010Performance All\u2010Organic Proton Batteries"],"prefix":"10.1002","volume":"65","author":[{"given":"Kang","family":"Guo","sequence":"first","affiliation":[{"name":"School of Chemical Science and Engineering State Key Laboratory of Cardiovascular Diseases and Medical Innovation Center Shanghai East Hospital Tongji University  Shanghai China"},{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-7510-5159","authenticated-orcid":false,"given":"Ziyang","family":"Song","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering State Key Laboratory of Cardiovascular Diseases and Medical Innovation Center Shanghai East Hospital Tongji University  Shanghai China"},{"name":"State Key Laboratory of Water Pollution Control and Green Resource Recycling College of Environmental Science and Engineering Advanced Research Institute Tongji University  Shanghai China"},{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3290-2116","authenticated-orcid":false,"given":"Qi","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Photovoltaic Science and Technology Institute of Optoelectronics College of Future Information Technology Fudan University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-0271-0010","authenticated-orcid":false,"given":"Zefeng","family":"Xu","sequence":"additional","affiliation":[{"name":"School of Chemical Science and Engineering State Key Laboratory of Cardiovascular Diseases and Medical Innovation Center Shanghai East Hospital Tongji University  Shanghai China"},{"name":"Shanghai Key Lab of Chemical Assessment and Sustainability  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0077-9048","authenticated-orcid":false,"given":"Yaokang","family":"Lv","sequence":"additional","affiliation":[{"name":"College of Chemical Engineering Zhejiang University of Technology  Hangzhou 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