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Herein, we propose a scaffold engineering strategy to construct an enzyme\u2013photo\u2013membrane coupled artificial photosynthetic system (\n                    <jats:italic>epm<\/jats:italic>\n                    CAPS) within HOF\u2010in\u2010HOF architecture for NADH regeneration and enzymatic hydrogenation, where enzyme\u2010loaded HOF particles for substrate conversion are encapsulated within photocatalytic HOF capsular membranes for cofactor regeneration. This unique configuration enables independent and synergistic regulation of electron, proton, and NADH transfer by modulating the electronic structure of the capsule (via benzene ring units), proton relay (via carboxylate group density), and mass diffusion path (via enzyme\u2013photocatalyst distance), respectively. The system achieves a record initial NADH regeneration rate of 28.23 \u00b1 0.62\u00a0mmol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a 22.13% apparent quantum yield. When applied to solar\u2010driven lactate synthesis, the\n                    <jats:italic>epm<\/jats:italic>\n                    CAPS achieves a solar\u2010to\u2010chemical conversion efficiency of 7.27 \u00b1 0.34%\u2014a nearly threefold higher than previous records. Furthermore, we demonstrate the generality of this platform by synthesizing a spectrum of C\n                    <jats:sub>1<\/jats:sub>\n                    \u2013C\n                    <jats:sub>6<\/jats:sub>\n                    chemicals, including methanol and mannitol, while maintaining stable operation for over 6\u00a0h. Our work delivers a blueprint for the next\u2010generation artificial photosynthetic systems for sustainable energy and green chemical production.\n                  <\/jats:p>","DOI":"10.1002\/anie.8868255","type":"journal-article","created":{"date-parts":[[2026,3,24]],"date-time":"2026-03-24T05:11:13Z","timestamp":1774329073000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Hydrogen\u2010Bonded Organic Frameworks (HOFs) for NADH Regeneration and Enzymatic Hydrogenation: HOF\u2010in\u2010HOF Artificial Photosynthetic System for Solar\u2010to\u2010Chemical Conversion"],"prefix":"10.1002","volume":"65","author":[{"given":"Wenping","family":"Li","sequence":"first","affiliation":[{"name":"Key Laboratory for Green Chemical Technology of the Ministry of Education, School of Chemical Engineering and Technology Tianjin University  Tianjin 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