Photocatalysis provides a new way for synchronous H2 production and organic synthesis at normal temperature and pressure, usually, water and organic substrate function as sources of hydrogen protons and organic products, which are complex and limited by two half-reactions. Employing alcohols as reaction substrates to simultaneously produce H2 and valuable organics in a redox cycle is worthy studying, to which catalyst design at atomic level holds the key. In this paper, Co elements doped Cu3P (CoCuP) quantum dots (QDs) are prepared and coupled with ZnIn2S4 (ZIS) nanosheets to form a 0D/2D p-n nanojunction which can effectively boost aliphatic and aromatic alcohols activation to simultaneously produce H2 and corresponding ketones (or aldehydes). The optimal CoCuP/ZIS composite demonstrated the highest activity for dehydrogenation of isopropanol to acetone (17.77 mmol⋅g-1⋅h-1) and H2 (26.8 mmol⋅g-1⋅h-1), which was 2.40 and 1.63 times higher than that of Cu3P/ZIS composite, respectively. Mechanistic investigations revealed that such high-performance originated from the accelerated electron transfer of the formed p-n junction and the thermodynamic optimization caused by the Co dopant which was the active site of oxydehydrogenation as a prerequisite step for isopropanol oxidation over the surface of the CoCuP/ZIS composite. Besides that, coupling of the CoCuP QDs can lower the dehydrogenation activation energy of isopropanol to form a key radical intermediate of (CH3)2CHO* for improving the activity of simultaneous production of H2 and acetone. This strategy provides an overall reaction strategy to obtain two meaningful products (H2 and ketones (or aldehydes)) and deeply explores the integrated redox reaction of alcohol as substrate for high solar-chemical energy conversion.