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Sustainable and scalable solar‐energy‐driven CO2 conversion into fuels requires earth‐abundant and stable photocatalysts. In this work, a defective Nb2C MXene as a cocatalyst and TiO2 microspheres as photo‐absorbers, constructed via a coulombic force‐driven self‐assembly, is synthesized. Such photocatalyst, at an optimized loading of defective Nb2C MXene (5% def‐Nb2C/TiO2), exhibits a CH4 production...