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Although structurally engineered g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    have shown promising photoinitiation performance, how modification\u2010induced changes in material properties affect their photoinitiation ability remains insufficiently understood. Herein, three g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    materials prepared through different structural and chemical modification strategies\u2014CN550 (prepared at 550\u00b0C), CN700 (thermally exfoliated), and TACN (tartaric acid\u2010assisted)\u2014are systematically compared as heterogeneous photoinitiators for visible\u2010light thiol\u2010ene photopolymerization. The comparative reveals that thermal exfoliation and tartaric acid\u2010assisted synthesis impart distinct advantages to g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    photoinitiators. CN700 exhibits consistently high photoinitiation ability across 405\u2013530\u00a0nm irradiation, benefiting from improved surface accessibility coupled with favorable optical and electronic properties, while TACN shows improved performance under longer\u2010wavelength irradiation due to its enhanced light\u2010harvesting capability. Efficient thiol\u2010ene photopolymerization is achieved in both organic and aqueous systems without additional co\u2010initiators, enabling one\u2010pot fabrication of composite materials. The optimized aqueous formulation is further explored to fabricate conductive hydrogels through NaCl incorporation, while the organic formulation enables direct laser writing for customized patterning. This work demonstrates that the photoinitiation ability of g\u2010C\n                    <jats:sub>3<\/jats:sub>\n                    N\n                    <jats:sub>4<\/jats:sub>\n                    relies on the combined effects of structural accessibility and photophysical properties, providing guidance for the design of semiconductor photoinitiators for visible\u2010light thiol\u2013ene photopolymerization.\n                  <\/jats:p>","DOI":"10.1002\/smll.75970","type":"journal-article","created":{"date-parts":[[2026,9,25]],"date-time":"2026-09-25T15:05:21Z","timestamp":1790348721000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Graphitic Carbon Nitride\u2010Based Photoinitiators for Multi\u2010Wavelength Thiol\u2010Ene Photopolymerization Toward Hydrogel Fabrication"],"prefix":"10.1002","author":[{"given":"Jun","family":"Shen","sequence":"first","affiliation":[{"name":"State Key Laboratory of High 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