Transition-metal　chalcogenides　(TMCs)　have　received　enormous　attention　by　virtue　of　their　large　light　absorption　coefficient,　abundant　catalytically　active　sites,　and　markedly　reduced　spatially　vectorial　charge-transfer　distance　originating　from　generic　structural　merits.　However,　the　controllable　construction　of　TMC-based　heterostructured　photosystems　for　photocatalytic　carbon　dioxide　(CO2)　reduction　is　retarded　by　the　ultrashort　charge　lifetime,　sluggish　charge-transfer　kinetics,　and　low　target　product　selectivity.　Herein,　we　present　the　rational　design　of　two-dimensional　(2D)/zero-dimensional　(0D)　heterostructured　CO2　reduction　photosystems　by　an　electrostatic　self-assembly　strategy,　which　is　enabled　by　precisely　anchoring　CsPbBr3　quantum　dots　(QDs)　on　the　2D　TMC　(CdIn2S4,　ZnIn2S4,　In2S3)　frameworks.　The　peculiar　2D/0D　integration　mode　and　suitable　energy-level　alignment　between　these　two　assembly　units　afford　maximal　interfacial　contact　and　applicable　potential　for　CO2　photoreduction,　thus　endowing　the　self-assembled　TMCs/CsPbBr3　nanocomposites　with　considerably　improved　visible-light-driven　photocatalytic　performances　toward　CO2　reduction　to　carbon　monoxide　with　high　selectivity.　The　enhanced　photocatalytic　performances　of　TMCs/CsPbBr3　heterostructures　are　attributed　to　the　abundant　active　sites　on　the　TMC　frameworks,　excellent　light　absorption　of　CsPbBr3　QDs,　and　well-defined　2D/0D　heterostructures　of　TMCs/CsPbBr3　QDs　photosystems,　which　synergistically　boosts　the　directional　charge　transport　from　CsPbBr3　QDs　to　TMCs,　enhancing　the　interfacial　charge　migration/separation.　Our　work　would　inspire　the　construction　of　novel　TMCs-involved　photosystems　for　solar-to-fuel　conversion.　©　2022　American　Chemical　Society.