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.