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Herein, a one‐step solvothermal method that shows incorporation of the graphene quantum dots (GQDs) on Fe‐based metal organic frameworks (MOFs) [MIL‐101(Fe)] to form GQD/MIL‐101(Fe) (G/M101) composites is reported. MIL‐101(Fe) with the sensitization of GQDs could significantly improve the photocatalytic reduction efficiency of CO2 to generate CO. The prepared composites exhibit excellent optical properties and the photocatalytic activity of G/M101 composites is relevant to GQDs ratio. The CO production rate over G/M101‐5% (224.71 µmol h−1 g−1) is 5 times higher than that of MIL‐101(Fe) (46.20 µmol h−1 g−1). The promising photocatalytic activity of G/M101‐5% strongly depends on the beneficial separation and transfer of photoinduced carriers via a charge migration between GQDs and MIL‐101(Fe). The microstructures and interfacial structures of the G/M101‐5% composite demonstrate that GQDs are closely loaded on the surface of MIL‐101 (Fe), and thus favors to the photoreduction according to their sp2 bonding. This work may figure a new way for the synthesis of photocatalysts for the application on carbon stabilization.

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