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Here, based on the stable mesoporous framework HOF\u2010102, \u03c0\u2010conjugation\u2010extended and donor\u2010acceptor\u2010tuned OBUs were predesigned by substituting the steric naphthalene units with benzene\u2010vinyl derivatives bearing \u2500H, \u2500CH\n                    <jats:sub>3<\/jats:sub>\n                    , or \u2500CN groups. Through a shape\u2010fitted \u03c0\u2500\u03c0 stacking strategy, three mesoporous HOFs isoreticular with HOF\u2010102 were synthesized from the tailored OBUs, namely HOF\u20101022, HOF\u20101022(CH\n                    <jats:sub>3<\/jats:sub>\n                    ), and HOF\u20101022(CN). These as\u2010synthesized HOFs exhibit pronounced variations in visible\u2010light absorption, with band gaps adjustable from 2.46 to 1.86\u00a0eV. Among these HOFs, the D\u2010A\u2010optimized HOF\u20101022(CN) possesses the narrowest band gap and exhibits significantly enhanced intraframework electron transfer and suppressed charge recombination, yielding an impressive hydrogen evolution activity of 168.2\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    , which is 8.5 times higher than that of HOF\u20101022(CH\n                    <jats:sub>3<\/jats:sub>\n                    ), and an apparent quantum yield (AQY) of 7.3% at 420\u00a0nm. This study represents the first demonstration of band\u2010gap engineering in HOFs materials and establishes a generalizable molecular\u2010design principle for developing high\u2010performance HOFs\u2010based photocatalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.202525987","type":"journal-article","created":{"date-parts":[[2026,2,3]],"date-time":"2026-02-03T07:08:53Z","timestamp":1770102533000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Band\u2010Gap Engineering of Isoreticular Hydrogen\u2010Bonded Organic Frameworks for Boosting Photocatalytic Hydrogen Evolution"],"prefix":"10.1002","volume":"65","author":[{"given":"Guanglai","family":"Mo","sequence":"first","affiliation":[{"name":"Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of Chemistry State Key Laboratory of Porous Materials For Separation and Conversion College of Smart Materials and Future Energy 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Pollution Control School of Light Industry and Food Engineering Guangxi University  Nanning China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiabao","family":"Liu","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Technology Hebei University of Technology  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qingyu","family":"Niu","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering and Technology Hebei University of Technology  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiangyu","family":"Gao","sequence":"additional","affiliation":[{"name":"Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials Department of Chemistry State Key Laboratory of Porous Materials For Separation and Conversion College of Smart Materials and Future Energy Fudan University  Shanghai 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