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While persistent charge availability post\u2010light cutoff is central to dark\u2010state catalysis, a quantitative structure\u2010dynamics\u2010function relationship linking molecular design to charge\u2010retention kinetics and post\u2010illumination reactivity remains unestablished. Here, we report a molecular tuning strategy of the central amine\u2010derived units that systematically regulates charge separation, retention timescales, and dark\u2010state H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production in imine\u2010linked polymer networks. Systematic evaluation of the series reveals a direct correlation between charge lifetime and dark activity. Compared with the N\u2010centered reference, the C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>3<\/jats:sub>\n                    \u2010centered analogue exhibits drastically prolonged electron\u2010associated transient lifetime, with a \u223c27\u2010fold longer decay timescale at the picosecond scale and a \u223c3\u2010fold increase at the nanosecond scale. This enhanced charge retention corresponds to a dark\u2010state H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production of 4941\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    within 40\u00a0min, \u223c1.5\u2010fold higher than that of the N\u2010centered counterpart. Density functional theory calculations reveal distinct electronic structures associated within the C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>3<\/jats:sub>\n                    \u2010centered framework, providing a favorable electronic environment for electron localization and subsequent utilization. These results establish a molecular structure\u2010charge retention\u2010dark reaction relationship for photocatalytic H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production beyond the illumination period.\n                  <\/jats:p>","DOI":"10.1002\/adma.75402","type":"journal-article","created":{"date-parts":[[2026,10,13]],"date-time":"2026-10-13T08:35:14Z","timestamp":1791880514000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecularly Modulated Charge Retention Enables Post\u2010Illumination H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Production in Imine\u2010Linked Polymers"],"prefix":"10.1002","author":[{"given":"Haishan","family":"Zhu","sequence":"first","affiliation":[{"name":"Beijing Key Lab of Microstructure and Property of Advanced Materials College of Materials and Engineering Beijing University of Technology  Beijing China"},{"name":"State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University  Xi'an China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yihong","family":"Zhang","sequence":"additional","affiliation":[{"name":"School of Materials and Chemical Engineering Henan University of Urban Construction  Pingdingshan China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-4326-9101","authenticated-orcid":false,"given":"Yijin","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Solidification Processing Center for Nano Energy Materials School of Materials Science and Engineering Northwestern Polytechnical University  Xi'an 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