Abstract Photo‐driven CH4 conversion to multi‐carbon products and H2 is attractive but challenging, and the development of efficient catalytic systems is critical. Herein, we construct a solar‐energy‐driven redox cycle for combining CH4 conversion and H2 production using iron ions. A photo‐driven iron‐induced reaction system was developed, which is efficient at selective coupling of CH4 as well as conversion of benzene and cyclohexane under mild conditions. For CH4 conversion, 94 % C2 selectivity and a C2H6 formation rate of 8.4 μmol h−1 is achieved. Mechanistic studies reveal that CH4 coupling is induced by hydroxyl radical, which is generated by photo‐driven intermolecular charge migration of an Fe3+ complex. The delicate coordination structure of the [Fe(H2O)5OH]2+ complex ensures selective C−H bond activation and C−C coupling of CH4. The produced Fe2+ can be used to reduce the potential for electrolytic H2 production, and then turns back into Fe3+, forming an energy‐saving and sustainable recyclable system.
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