Inspired by the unique structure and wide applications of zeolitic imidazolate frameworks-8 (ZIF-8) and CuInS2 (CIS), considerable attention has focused on the combination of both materials. We herein report a facial method for the homogeneous decoration of ZIF-8 onto the surfaces of CuInS2 (CIS) nanoparticles coordinated by polyvinyl pyrrolidone (PVP) in methanol. It has been shown that the coordination of PVP plays a key role in inducing the nucleation of ZIF-8 on the surface of CIS nanoparticles because of the pyrrolidone rings (C = 0) in PVP offering an improved affinity between CIS and Zn ions. Performing as a catalyst, the CIS@ZIF-8 nanocomposites not only exhibit high photocatalytic activity for the degradation of organic dye under UV light irradiation, but also largely maintain their catalytic efficiency after being recycled for five times compared with that of pure CIS nanoparticles.