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Herein, two van der Waals heterojunctions were constructed by integrating ultrathin poly(triazine imide) (PTI) nanosheets with two structurally distinct covalent organic frameworks (COFs), giving rise to distinct interfacial growth behaviors for TTB\u2010COF and TTT\u2010COF on the PTI surface. Compared with the lateral (face\u2010to\u2010face) stacking in PTI\u2010TTT, the predominantly vertical interfacial contact in PTI\u2010TTB is associated with a more intimate interface, stronger internal electric field, and more abundant accessible active sites. As a result, the optimized PTI\u2010TTB delivers a superior H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    production rate of 4402\u2009\u03bcmol\u2009g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u2009h\n                    <jats:sup>\u22121<\/jats:sup>\n                    with an apparent quantum yield of 2.61% at 420\u2009nm, which are 23.4 and 4.8 times higher than those of pristine PTI and TTB\u2010COF, respectively. Experimental results and density functional theory (DFT) calculations support that the superior photocatalytic performance is related to an efficient S\u2010scheme charge transfer pathway established at the strongly coupled interface. Mechanistic investigations further indicate that the synergistic coupling of the two\u2010electron oxygen reduction reaction (2e\n                    <jats:sup>\u2212<\/jats:sup>\n                    ORR) and two\u2010electron water oxidation reaction (2e\n                    <jats:sup>\u2212<\/jats:sup>\n                    WOR) accounts for the enhanced H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    photosynthesis.\n                  <\/jats:p>","DOI":"10.1002\/cssc.70976","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T12:38:07Z","timestamp":1786538287000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Vertical Growth of Covalent Organic Frameworks on Poly(triazine imide) Nanosheets: Constructing an Efficient S\u2010Scheme van der Waals Heterojunction for H\n                    <sub>2<\/sub>\n                    O\n                    <sub>2<\/sub>\n                    Photosynthesis"],"prefix":"10.1002","volume":"19","author":[{"given":"Yizhao","family":"Liang","sequence":"first","affiliation":[{"name":"Hebei Key Laboratory of Inorganic Nano\u2010materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ziyi","family":"Li","sequence":"additional","affiliation":[{"name":"Hebei Key Laboratory of Inorganic Nano\u2010materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zixuan","family":"Li","sequence":"additional","affiliation":[{"name":"Hebei Key Laboratory of Inorganic Nano\u2010materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 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