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Conventional strategies have focused on intrinsic electronic structure optimization of active sites while overlooking the critical influence of the reaction microenvironment on coupling probability. Herein, we propose a dynamic soft\u2010confinement catalytic strategy by in situ constructing a disordered hydrogen\u2010bonded organic framework (HOF) layer on Bi\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    Br surfaces, thereby establishing an HOF\/Bi\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    Br integrated photocatalytic system. The introduction of HOF not only induces the formation of asymmetric Bi\n                    <jats:sub>1<\/jats:sub>\n                    \u2013Bi\n                    <jats:sub>2<\/jats:sub>\n                    coupling sites but also establishes a dynamic hydrogen\u2010bonding microenvironment surrounding them. This microenvironment enhances CO\n                    <jats:sub>2<\/jats:sub>\n                    coverage near the coupling sites by constructing a persistent carbon source enrichment layer. Simultaneously, the interfacial polarization field promotes exciton dissociation and directs electron transport toward the Bi\n                    <jats:sub>1<\/jats:sub>\n                    \u2013Bi\n                    <jats:sub>2<\/jats:sub>\n                    sites. Furthermore, the reconfigurable hydrogen bonds impose orientational soft confinement on *CO intermediates, guiding them into spatial configurations favorable for *OCCO bond formation. This soft\u2010hard synergistic interfacial design enables 0.7HOF\/Bi\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>4<\/jats:sub>\n                    Br to achieve a CH\n                    <jats:sub>3<\/jats:sub>\n                    COOH production rate of 325.12\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with 98.81% product selectivity under sacrificial agent\u2010free conditions. This work demonstrates that dynamic microenvironment programming around active sites constitutes a critical pathway for overcoming the photocatalytic C\u2013C coupling bottleneck.\n                  <\/jats:p>","DOI":"10.1002\/anie.5407135","type":"journal-article","created":{"date-parts":[[2026,10,17]],"date-time":"2026-10-17T06:10:48Z","timestamp":1792217448000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Dynamic Soft\u2010Confinement via Hydrogen\u2010Bonded Organic Frameworks Reshapes C\u2013C Coupling Interfacial Chemistry at Bi\n                    <sub>1<\/sub>\n                    \u2013Bi\n                    <sub>2<\/sub>\n                    Sites"],"prefix":"10.1002","author":[{"given":"Zhiwei","family":"Shao","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering National Special Superfine Powder Engineering Research Center Nanjing University of Science and Technology  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9197-8922","authenticated-orcid":false,"given":"Caichao","family":"Ye","sequence":"additional","affiliation":[{"name":"Academy for Advanced Interdisciplinary Studies &amp; Department of Materials Science and Engineering Guangdong Provincial Key Laboratory of Computational Science and Material Design Southern University of Science and Technology  Shenzhen P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0596-7232","authenticated-orcid":false,"given":"Jun","family":"Xiong","sequence":"additional","affiliation":[{"name":"Institute for Energy Research Jiangsu University  Zhenjiang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaojing","family":"Bi","sequence":"additional","affiliation":[{"name":"School of Chemistry and Chemical Engineering National Special Superfine Powder Engineering Research Center Nanjing University of Science and Technology  Nanjing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xuhao","family":"Yang","sequence":"additional","affiliation":[{"name":"MIIT Key Laboratory of Advanced Display Material and Devices School of Materials Science and Engineering Nanjing University of Science and Technology  Nanjing P. R. 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