Solar-powered interfacial water evaporation technology coupled with photocatalytic function is considered as a promising solution to achieve the dye wastewater purification and solve the problem of organic pollution’s enrichment on traditional solar absorbers. In this study, a two-dimensional (2D) MoS2/ZnIn2S4 composite was designed by a two-step hydrothermal method, and served as a solar absorber with a water evaporation rate of 1.54 kgꞏm−2ꞏh−1. The deposition of ZnIn2S4 on MoS2 endowed the composite with 98.7% of photodegradation efficiency for dye wastewater via the construction of type Ⅰ heterojunction and avoided the problem of secondary pollution of dye wastewater. This study successfully integrated photocatalysis into the cutting-edge solar-driven interfacial evaporation system, accomplishing the expansion of multifunctional solar absorber and extending the application for the treatment of dye wastewater with zero wastewater discharge.