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Herein, we develop a molten\u2010salt\u2010induced defect engineering on ultrathin carbon nitride (CNx) to enable highly efficient pure\u2010water H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    photosynthesis via a dual\u2010channel two\u2010electron oxygen reduction reaction (ORR) and water oxidation reaction (WOR) pathway. The CNx catalyst delivers a record H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production rate of 1100.9\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    under pure water conditions without sacrificial agents. Mechanistically, transient photovoltage (TPV) and transient potential scan (TPS) quantitatively elucidate that defect sites expedite charge separation, mitigate deep trap states, and accelerate light\u2010induced oxygen activation kinetics rather than merely enhancing oxygen adsorption. Crucially, we translate this system into a practical continuous\u2010flow architecture by encapsulating CNx within a sodium alginate hydrogel matrix (CNx\/SA). This hydrogel flow reactor sustains a stable H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production of 180\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    h\n                    <jats:sup>\u22121<\/jats:sup>\n                    over 400 h. Furthermore, a multiphysics mathematical framework validates that the hydrogel microenvironment fundamentally suppresses degradation pathways and facilitates product desorption. This study provides a comprehensive paradigm integrating atomic\u2010level catalyst design with macroscopic reactor engineering for scalable solar\u2010driven chemical manufacturing.\n                  <\/jats:p>","DOI":"10.1002\/smll.75968","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T16:49:56Z","timestamp":1790527796000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Coupling Light\u2010Heat Utilization in Hydrogel\u2010Encapsulated Ultrathin Defective Carbon Nitride Nanosheets for Scalable Continuous\u2010Flow H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Photosynthesis"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-3989-3905","authenticated-orcid":false,"given":"Zhongshan","family":"Yang","sequence":"first","affiliation":[{"name":"Sino\u2010Luso Joint Laboratory for 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