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Herein, we first report a new strategy of in situ constructing oriented COF\u2010based PN heterostructure film through single\u2010layer MoS\n                    <jats:sub>2<\/jats:sub>\n                    induced growth, significantly enhancing the photogenerated carrier separation efficiency, which promotes the photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    synthesis. Experimental results reveal that the as\u2010made oriented TAPB\u2010DMTA COF\/MoS\n                    <jats:sub>2<\/jats:sub>\n                    (TAPB: 1,3,5\u2010tris(4\u2010aminophenyl) benzene, DMTA: 2,5\u2010Dimethoxyterephthalaldehyde) film exhibits a high photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    yield of 8154 \u00b5mol\u00a0g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , which is \u223c2.5 times and \u223c4 times higher than that of non\u2010oriented TAPB\u2010DMTA COF films and powder. The mechanism reveals that the oriented structure of the TAPB\u2010DMTA COF can significantly promote the generation and the transmission of photogenerated electron\u2010hole pairs along the skeleton and layer\u2010by\u2010layer stacking direction, thus enhancing the photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    performance. The new strategy of in situ constructing oriented COFs\u2010based PN heterostructure film for enhancing the photosynthesis of H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    will open the door to rational design of molecular films towards high photogenerated carrier separation efficiency.\n                  <\/jats:p>","DOI":"10.1002\/anie.202505491","type":"journal-article","created":{"date-parts":[[2025,4,15]],"date-time":"2025-04-15T01:02:06Z","timestamp":1744678926000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":30,"title":["Constructing Large\u2010Area Oriented Covalent Organic Framework Based PN Heterostructure Films to Enhance Artificial Photosynthesis of H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>"],"prefix":"10.1002","volume":"64","author":[{"given":"Minghui","family":"Liu","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P.R. 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China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wenqiang","family":"Gao","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P.R. China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyu","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences  Beijing 100190 P.R. China"},{"name":"University of Chinese Academy of Sciences  Beijing 100049 P.R. 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