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Photocatalytic reduction of CO2 has drawn much attention as a promising way that can effectively alleviate the issue of global warming and energy crisis. In this work, we fabricated a series of CdS/NH2‐UiO‐66 composites with varied CdS amounts and tested their capacity for photocatalytic reduction of CO2. The reactions were performed in a solvent‐free system and displayed excellent selectivity for CO production without liquid phase products. When the content of CdS in the composite is up to 40 %, the hybrid catalyst produces 105.41 μmol/g within 6 h, exhibiting remarkable photocatalytic performance, which is much higher than that catalyzed by mechanically mixed CdS and NH2‐UiO‐66. The brilliant catalytic performance of the composite catalyst is attributed to the formation of heterostructure between the well‐dispersed CdS and NH2‐UiO‐66, which promotes the enhancement of electron transfer during photocatalysis. [ABSTRACT FROM AUTHOR]