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Quantum dots (QDs), a class of promising candidates for harvesting visible light, generally exhibit low activity and selectivity towards photocatalytic CO₂ reduction. Functionalizing QDs with metal complexes (or metal cations through ligands) is a widely used strategy for improving their catalytic activity; however, the resulting systems still suffer from low selectivity and stability in CO₂ reduction. Herein, we report that doping CdS QDs with transition‐metal sites can overcome these limitations and provide a system that enables highly selective photocatalytic reactions of CO₂ with H₂O (100 % selectivity to CO and CH₄), with excellent durability over 60 h. Doping Ni sites into the CdS lattice leads to effective trapping of photoexcited electrons at surface catalytic sites and substantial suppression of H₂ evolution. The method reported here can be extended to various transition‐metal sites, and offers new opportunities for …