Precise　regulation　and　control　solar-light-driven　charges　photoexcited　on　photocatalysts　for　separation-transfer　and　target　redox　reactions　is　an　attractive　and　challenging　pathway　toward　sustainability.　Herein,　0D/2D-3D　Pt/In2S3　Schottky　junction　was　fabricated　for　simultaneous　selective　phenylcarbinol　conversion　into　value-added　aldehydes　and　production　of　clean　energy　H2　by　directly　utilizing　photoexcited　holes　and　electrons　in　one　reaction　system　under　mild　reaction　conditions.　In　contrast　to　pure　water　splitting　and　pure　In2S3,　the　reaction　thermodynamics　and　kinetics　of　H2　evolution　on　the　Pt/In2S3　were　significantly　enhanced.　The　optimized　0.3%　Pt/In2S3　exhibited　the　highest　and　most　stable　photocatalytic　activity　with　22.1　mmol　g−1　h−1　of　H2　production　rate　and　almost　100%　selectivity　of　benzaldehyde　production.　Notably,　this　dual-function　photocatalysis　also　exhibited　superiority　in　contrast　to　sacrificial-agent　H2　evolution　reactions　such　as　lactic　acid,　Na2S,　methanol　and　triethanolamine.　The　turnover　frequency　(TOF)　could　reach　up　to　~2394　h−1.　The　Pt　clusters　anchored　at　the　electron　location　and　strong　metal-support　interactions　(SMSI)　between　Pt　and　In2S3　synergistically　improved　the　spatial　charge　separation　and　directional　transportation　(~90.1%　of　the　charge　transport　efficiency　could　be　achieved　over　the　Pt/In2S3　hybrid),　and　thus　result　in　significant　enhancement　of　photocatalytic　H2　evolution　with　simultaneous　benzaldehyde　production.　©　2023　by　the　authors.