The morphology, chemical composition, and doping process of metal oxides and sulfides play a significant role in their photocatalytic performance under solar light illumination. We synthesized Cu2+-doped ZnO–SnS nanocomposites at 220 °C for 10 h, using hydrothermal methods. These nanocomposites were structurally, morphologically, and optically characterized using various techniques, including powder X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and UV-visible absorption spectroscopy. Their photocatalytic activity (PCA) on methylene blue (MB) pollutant dye was examined under 150 W solar light illumination. Mixed-phase abundances with hexagonal ZnO and orthorhombic SnS structures were observed. TEM micrographs showed changes in morphology from spherical to nano-flake structures with an increasing doping concentration. XPS indicated the chemical states of the constituent elements in the nanocomposites. UV-visible absorption spectroscopy showed a decrease in the bandgap with an increasing doping concentration. Strong PCA was observed due to the separation of charge carriers, a change in bandgap, and a high light absorption ability under solar light irradiation. The measured photodegradation efficiency of the MB dye was approximately 97% after 2 h. The movement of the charge carriers and the bandgap alignment of the synthesized composites are briefly discussed.