AbstractHigh-performance and low-cost photocatalysts play the key role in achieving the large-scale solar hydrogen production. In this work, we report a liquid-exfoliation approach to prepare NiPS₃ ultrathin nanosheets as a versatile platform to greatly improve the light-induced hydrogen production on various photocatalysts, including TiO₂, CdS, In₂ZnS₄ and C₃N₄. The superb visible-light-induced hydrogen production rate (13,600 μmol h⁻¹ g⁻¹) is achieved on NiPS₃/CdS hetero-junction with the highest improvement factor (~1,667%) compared with that of pure CdS. This significantly better performance is attributed to the strongly correlated NiPS₃/CdS interface assuring efficient electron-hole dissociation/transport, as well as abundant atomic-level edge P/S sites and activated basal S sites on NiPS₃ ultrathin nanosheets advancing hydrogen evolution. These findings are revealed by the state-of-art characterizations and theoretical computations. Our work for the first time demonstrates the great potential of metal phosphorous chalcogenide as a general platform to tremendously raise the performance of different photocatalysts.