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We transcend incremental catalyst optimization by introducing a universal molecular design strategy \u201csimultaneous geometric and electronic symmetry breaking\u201d in covalent organic frameworks that intrinsically programs directional charge flow. Our strategy of replacing symmetric benzene units with asymmetric thiophene rings induces cooperative point\u2010group distortion and asymmetric electron density redistribution, thereby creating a built\u2010in polarization field that slashes exciton binding energy, extends carrier lifetime by over 300%, and steers reaction selectivity. This leads to a record photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production rate from just water and air. Crucially, life\u2010cycle assessment confirms this pathway reduces environmental impact by an order of magnitude. The generality of this design strategy is further validated across multiple framework systems and enables stable operation in a continuous\u2010flow photoreactor, demonstrating a robust platform for efficient solar\u2010to\u2010chemical energy conversion.\n                  <\/jats:p>","DOI":"10.1002\/anie.4908536","type":"journal-article","created":{"date-parts":[[2026,5,31]],"date-time":"2026-05-31T16:20:03Z","timestamp":1780244403000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Dual Breaking the Geometric and Electronic Symmetry of Covalent Organic Framework for Enhanced H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Photosynthesis"],"prefix":"10.1002","volume":"65","author":[{"given":"Qiang","family":"Xue","sequence":"first","affiliation":[{"name":"State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian P. 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