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Here, we report conjugated bithiophene frameworks (CBFs) that integrate molecularly differentiated redox motifs with alkynyl\u2010regulated electron\u2013proton coordination for efficient H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    photosynthesis. Progressive extension of alkynyl bridges from CBF\u2010TB to CBF\u2010TDB induces an intraframework excited\u2010state redox polarization that biases photogenerated holes toward benzene\/alkynyl motifs and electrons toward thiophene units, facilitating water oxidation and oxygen reduction, respectively. Simultaneously, the alkynyl\u2010rich framework organizes interfacial water into a hydrogen\u2010bonded network that facilitates proton delivery to the oxygen reduction interface. The resulting synergy between directional charge transport and localized proton supply promotes proton\u2010coupled two\u2010electron oxygen reduction to H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    . Consequently, CBF\u2010TDB achieves a solar\u2010to\u2010chemical conversion efficiency of 1.01% under simulated solar irradiation, more than 4 times that of the alkynyl\u2010free analogue CBF\u2010TB (0.21%). This study establishes the coordinated regulation of excited\u2010state charge polarization and interfacial proton delivery as a molecular design principle for efficient H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    photosynthesis and, more broadly, multistep solar\u2010to\u2010chemical conversions.\n                  <\/jats:p>","DOI":"10.1002\/anie.3374480","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T10:16:31Z","timestamp":1788776191000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coordination of Electron Transfer and Proton Supply in Conjugated Polymer Frameworks for Efficient Hydrogen Peroxide 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