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Herein, we construct a solar\u2010energy\u2010driven redox cycle for combining CH<jats:sub>4<\/jats:sub> conversion and H<jats:sub>2<\/jats:sub> production using iron ions. A photo\u2010driven iron\u2010induced reaction system was developed, which is efficient at selective coupling of CH<jats:sub>4<\/jats:sub> as well as conversion of benzene and cyclohexane under mild conditions. For CH<jats:sub>4<\/jats:sub> conversion, 94\u2009% C<jats:sub>2<\/jats:sub> selectivity and a C<jats:sub>2<\/jats:sub>H<jats:sub>6<\/jats:sub> formation rate of 8.4\u2005\u03bcmol\u2009h<jats:sup>\u22121<\/jats:sup> is achieved. Mechanistic studies reveal that CH<jats:sub>4<\/jats:sub> coupling is induced by hydroxyl radical, which is generated by photo\u2010driven intermolecular charge migration of an Fe<jats:sup>3+<\/jats:sup> complex. The delicate coordination structure of the [Fe(H<jats:sub>2<\/jats:sub>O)<jats:sub>5<\/jats:sub>OH]<jats:sup>2+<\/jats:sup> complex ensures selective C\u2212H bond activation and C\u2212C coupling of CH<jats:sub>4<\/jats:sub>. The produced Fe<jats:sup>2+<\/jats:sup> can be used to reduce the potential for electrolytic H<jats:sub>2<\/jats:sub> production, and then turns back into Fe<jats:sup>3+<\/jats:sup>, forming an energy\u2010saving and sustainable recyclable system.<\/jats:p>","DOI":"10.1002\/anie.202303405","type":"journal-article","created":{"date-parts":[[2023,4,22]],"date-time":"2023-04-22T04:13:13Z","timestamp":1682136793000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":27,"title":["Photo\u2010Driven Iron\u2010Induced Non\u2010Oxidative Coupling of Methane to Ethane"],"prefix":"10.1002","volume":"62","author":[{"given":"Huizhen","family":"Zhang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Physical Chemistry of Solid Surfaces Collaborative Innovation Center of Chemistry for Energy Materials National Engineering Laboratory for Green Chemical Productions of Alcohols Ethers and Esters College of Chemistry and Chemical Engineering Xiamen University  Xiamen 361005 Fujian P. 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