The reasonable design and fabrication of heterojunction could regulate the photocatalytic performance to some extent, yet it is still a great challenge to construct the S-scheme heterostructure with the stable as well as tight interface on the surface of semiconductor photocatalysts. Herein, the ZnIn₂S₄/Cu₂MoS₄ (ZIS/CMS) S-scheme heterostructure was fabricated by in-situ assembling ZIS nanosheets on the CMS plates, obtaining a mossy tile-like morphology. Owing to the compact interface resulting from in-situ growth, this unique architecture efficiently facilitated the separation and transfer of light-induced charges, guaranteed the larger interface area, and enriched the active sites for photocatalytic redox reactions. After adjusting the mass ratio of CMS in ZIS/CMS, S-scheme heterostructure exhibited the remarkable performance with an optimal H₂ producing rate up to 1298 μmol·h⁻¹ g⁻¹, about 13.8 times than that of pristine ZIS. The mechanism and driving force of charge transfer and separation in S-scheme heterostructure photocatalysts were explained and discussed. This investigation will provide new insight into design and construction of S-scheme heterojunction photocatalysts for H₂ evolution.