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Here, we present a supramolecular approach to defect engineering within a soft hydrogel matrix by confining a Bi\n                    <jats:sup>3+<\/jats:sup>\n                    \u2010caffeic acid complex within a guanosine monophosphate\u2010based G\u2010quadruplex hydrogel. This confinement not only breaks local coordination symmetry and generates oxygen\u2010vacancy\u2010rich heterojunctions but also emulates the active\u2010site environments of enzymes. The G\u2010quadruplex fibrillar scaffold provides ion\u2010channel\u2010like pathways that facilitate charge transport, enhance substrate diffusion, and promote selective adsorption, while confinement ensures the uniform dispersion of catalytic sites. Together, these synergistic effects result in an exceptional N\n                    <jats:sub>2<\/jats:sub>\n                    to NH\n                    <jats:sub>3<\/jats:sub>\n                    conversion of 905.2\u00a0\u00b5mol h\n                    <jats:sup>\u22121<\/jats:sup>\n                    g\n                    <jats:sup>\u22121<\/jats:sup>\n                    <jats:sub>(cat)<\/jats:sub>\n                    under visible light irradiation, 3.8 times higher than that of the pristine complex. This work introduces a versatile strategy that integrates defect engineering, heterojunction formation, and biomimetic confinement within a soft supramolecular assembly, establishing G\u2010quadruplex hydrogels as a powerful platform for sustainable photocatalytic nitrogen fixation and beyond.\n                  <\/jats:p>","DOI":"10.1002\/smll.202514925","type":"journal-article","created":{"date-parts":[[2026,2,19]],"date-time":"2026-02-19T08:46:42Z","timestamp":1771490802000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Intermingled Coordination Environments Enable Defect\u2010Engineered Metal\u2013Polyphenol\/G\u2010Quadruplex Hydrogel for Enhanced N\n                    <sub>2<\/sub>\n                    \u2010to\u2010NH\n                    <sub>3<\/sub>\n                    Photoconversion"],"prefix":"10.1002","volume":"22","author":[{"ORCID":"https:\/\/orcid.org\/0009-0005-9023-0700","authenticated-orcid":false,"given":"Tarun Kumar","family":"Sahu","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Indore Madhya Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shaurya","family":"Aneja","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Indore Madhya Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-6097-8526","authenticated-orcid":false,"given":"Ravindra","family":"Vishwakarma","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Indore  Indore Madhya Pradesh 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