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The molecular junction strategy has been proven to be an effective approach to address the aforementioned challenges. In this work, we developed a molecular junction through controlled thermal ring\u2010opening isomerization of benzoguanamine, thereby creating a well\u2010defined C\u2010C\u2010bridged benzene\u2010heptazine molecular junction. Experimental and theoretical studies reveal that: (1) Benzene functionalization extends the \u03c0\u2010conjugation, enabling n\u2192\u03c0* transitions for broad\u2010spectrum absorption; (2) The donor\u2010acceptor structure enhances self\u2010polarization effects, strengthening the built\u2010in electric field for efficient charge separation; (3) The unique molecular architecture overcomes traditional kinetic limitations, enabling a dual\u2010channel H\n                    <jats:sub>2<\/jats:sub>\n                    O\n                    <jats:sub>2<\/jats:sub>\n                    synthesis mechanism. The optimized catalyst achieves remarkable production rates of 5222 \u00b5mol\u2219g\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    \u2219h\n                    <jats:sup>\u2212<\/jats:sup>\n                    <jats:sup>1<\/jats:sup>\n                    in isopropanol\/water and 1587 \u00b5mol\u2219g\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u2219h\n                    <jats:sup>\u22121<\/jats:sup>\n                    in pure water, representing 13.1\u2010fold and 32.4\u2010fold improvements over pristine CN, respectively. This work advances molecular\u2010scale design of photocatalysts and offers new strategies for artificial photosynthesis.\n                  <\/jats:p>","DOI":"10.1002\/smll.74758","type":"journal-article","created":{"date-parts":[[2026,7,23]],"date-time":"2026-07-23T09:46:08Z","timestamp":1784799968000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Molecular Benzene\u2010Heptazine Junction Over Carbon Nitride Frameworks for Dual\u2010Pathway Photosynthesis of Hydrogen Peroxide"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-4131-0737","authenticated-orcid":false,"given":"Yuanyuan","family":"Liu","sequence":"first","affiliation":[{"name":"School of Materials and Chemical Engineering Xuzhou University of Technology  Xuzhou Jiangsu 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