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Here, we report a metal\u2010free graphdiyne (GDY)\/polymeric carbon nitride (PCN) heterojunction that achieves exceptional bifunctional performance in CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction coupled with tetrahydrofuran oxidation to\n                    <jats:italic>\u03b3<\/jats:italic>\n                    \u2010butyrolactone. The optimized composite delivers a CO production rate of 55 \u00b5mol\u00b7h\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00b7g\n                    <jats:sup>\u22121<\/jats:sup>\n                    with 95% selectivity, and a\n                    <jats:italic>\u03b3<\/jats:italic>\n                    \u2010butyrolactone yield of 54% with near\u2010unity selectivity (&gt; 99%) under mild photothermal conditions, representing 2.9\u2010fold and 6.8\u2010fold enhancements over thermally treated PCN, respectively. Mechanistic investigations reveal that GDY serves as a hole\u2010transport layer, generating a built\u2010in electric field that drives spatial separation of charge carriers. This configuration confines electrons on PCN for CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction while directing holes to GDY for tetrahydrofuran activation. Moreover, the metal\u2010free heterojunction suppresses over\u2010oxidation pathways that plague metal\u2010loaded systems, enabling remarkable selectivity control. This work establishes the GDY\/PCN heterojunction as a powerful platform for cooperative photoredox catalysis and provides a blueprint for designing metal\u2010free heterojunctions toward sustainable synthesis.\n                  <\/jats:p>","DOI":"10.1002\/anie.3147768","type":"journal-article","created":{"date-parts":[[2026,5,18]],"date-time":"2026-05-18T03:20:59Z","timestamp":1779074459000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Graphdiyne as a Hole\u2010Transport Channel in Carbon Nitride Heterojunctions for Synergistic CO\n                    <sub>2<\/sub>\n                    Reduction and\n                    <i>\u03b3<\/i>\n                    \u2010Butyrolactone Synthesis"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-3465-7118","authenticated-orcid":false,"given":"Xuan","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemistry for NBC Hazards Protection State Key Laboratory of Photocatalysis on Energy and Environment Sino\u2010UK International Joint Laboratory on Photocatalysis for Clean Energy and Advanced Chemicals &amp; Materials College of Chemistry Fuzhou University  Fuzhou P. 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