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Herein, we pioneer a radical\/active\u2010site synergistic strategy to steer the reaction pathway exclusively toward methanol. This is realized by a dual\u2010functional Cl\u2500TiO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010OV catalyst that integrates chlorine modification and oxygen vacancy (OV) engineering. Crucially, surface chlorine redirects the oxidation route: instead of generating non\u2010selective \u2022OH radicals from H\n                    <jats:sub>2<\/jats:sub>\n                    O, photogenerated holes preferentially drive a Cl\n                    <jats:sup>\u2212<\/jats:sup>\n                    \/Cl\u2022 cycle. The resulting Cl\u2022 radicals activate the C\u2500H bond of CH\n                    <jats:sub>4<\/jats:sub>\n                    to form \u2022CH\n                    <jats:sub>3<\/jats:sub>\n                    , which combines with O\n                    <jats:sub>2<\/jats:sub>\n                    to yield the CH\n                    <jats:sub>3<\/jats:sub>\n                    OOH intermediate. Simultaneously, the engineered OV sites act as electron\u2010rich centers that efficiently reduce CH\n                    <jats:sub>3<\/jats:sub>\n                    OOH to CH\n                    <jats:sub>3<\/jats:sub>\n                    OH. This decoupling of selective oxidation (via Cl\u2022) and efficient reduction (via OVs) suppresses all side\u2010reactions, delivering methanol with nearly 100% selectivity and a yield of 1242\u00a0\u00b5mol g\n                    <jats:sup>\u22121<\/jats:sup>\n                    . In contrast, TiO\n                    <jats:sub>2<\/jats:sub>\n                    \u2010OV suffers from \u2022OH\u2010mediated sequential oxidation to HCHO\/CO\n                    <jats:sub>2<\/jats:sub>\n                    , and Cl\u2500TiO\n                    <jats:sub>2<\/jats:sub>\n                    lacks sufficient reduction power, resulting in a CH\n                    <jats:sub>3<\/jats:sub>\n                    OOH\/CH\n                    <jats:sub>3<\/jats:sub>\n                    OH mixture. This work not only offers an effective approach for highly selective photocatalytic methane conversion but also deepens mechanistic insight into radical\/active\u2010site cooperativity in synergistic catalysis.\n                  <\/jats:p>","DOI":"10.1002\/anie.3983956","type":"journal-article","created":{"date-parts":[[2026,5,18]],"date-time":"2026-05-18T03:13:12Z","timestamp":1779073992000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":3,"title":["Near\u2010100% Selective Photocatalytic Methane\u2010to\u2010Methanol Conversion Enabled by Synergistic Chlorine Radicals and Oxygen Vacancies"],"prefix":"10.1002","volume":"65","author":[{"given":"Guang\u2010Xing","family":"Dong","sequence":"first","affiliation":[{"name":"State Key Laboratory of Crystal Materials Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystals Tianjin University of Technology  Tianjin China"},{"name":"Institute For New Energy Materials and Low Carbon Technologies School of Electrical Engineering and Automation Tianjin University of Technology  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Min","family":"Zhang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Crystal Materials Tianjin Key Laboratory of Functional Crystal Materials Institute of Functional Crystals Tianjin University of Technology  Tianjin China"},{"name":"Institute For New Energy Materials and Low Carbon Technologies School of Electrical Engineering and Automation Tianjin University of Technology  Tianjin China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ting","family":"Zheng","sequence":"additional","affiliation":[{"name":"Institute For New Energy Materials and Low Carbon Technologies School of Electrical Engineering and Automation Tianjin University of Technology  Tianjin 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