Semiconductor　quantum　dots　have　been　emerging　as　one　of　the　most　ideal　materials　for　artificial　photosynthesis.　Here,　we　report　the　assembled　ZnS-CdS　hybrid　heterostructure　for　efficient　coupling　cooperative　redox　catalysis　toward　the　oxidation　of　1-phenylethanol　to　acetophenone/2,3-diphenyl-2,3-butanediol　(pinacol)　integrated　with　the　reduction　of　protons　to　H2.　The　strong　interaction　and　typical　type-I　band-position　alignment　between　CdS　quantum　dots　and　ZnS　quantum　dots　result　in　efficient　separation　and　transfer　of　electron-hole　pairs,　thus　distinctly　enhancing　the　coupled　photocatalyzed-redox　activity　and　stability.　The　optimal　ZnS-CdS　hybrid　also　delivers　a　superior　performance　for　various　aromatic　alcohol　coupling　photoredox　reaction,　and　the　ratio　of　electrons　and　holes　consumed　in　such　redox　reaction　is　close　to　1.0,　indicating　a　high　atom　economy　of　cooperative　coupling　catalysis.　In　addition,　by　recycling　the　scattered　light　in　the　near　field　of　a　SiO2　sphere,　the　SiO2-supported　ZnS-CdS　(denoted　as　ZnS-CdS/SiO2)　catalyst　can　further　achieve　a　3.5-fold　higher　yield　than　ZnS-CdS　hybrid.　Mechanistic　research　clarifies　that　the　oxidation　of　1-phenylethanol　proceeds　through　the　pivotal　radical　intermediates　of　•C(CH3)(OH)Ph.　This　work　is　expected　to　promote　the　rational　design　of　semiconductor　quantum　dots-based　heterostructured　catalysts　for　coupling　photoredox　catalysis　in　organic　synthesis　and　clean　fuels　production.　©　2023　Lin-Xing　Zhang　et　al.