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• SnS 2 atomic layer with Pt 3 Co nanoclusters have been successfully prepared. • Nanoclusters can enrich electrons, reduce barriers, and promote proton transport. • The photoelectric properties of catalysts is significantly enhanced. • The CO 2 photoreduction efficiency of the SnS 2 /Pt 3 Co catalyst is markedly improved. Poor capability of charge-holes separation and slower surface CO 2 reaction kinetics hinder photocatalytic performance. Here, SnS 2 atomic layer with Pt 3 Co alloy nanoclusters have been successfully prepared. Nanoclusters could be used as highly catalytic active sites, which not only facilitates the carrier separation and transport kinetics, but enriches electrons lowered the reaction barrier. As expected, the CO evolution rate of the champion SnS 2 /Pt 3 Co catalyst was 13.6 times higher than that of the original SnS 2 catalyst under white light irradiation. In-situ DRIFTS identifies key intermediate in the photoreduction process. In-situ XPS and DFT calculation further verifies the electron transport direction and charge density distribution at the SnS 2 /Pt 3 Co interface. Our work uncovers the role of nanoclusters in carrier separation and transport as well as proton transport, opening new chances for obtaining efficient photoreduction CO 2 property. [ABSTRACT FROM AUTHOR]