Copper sulfide and zinc sulfide nanostructures were synthesized using a solvo/hydrothermal method and a thio Schiff base ligand, N‐benzylidene ethanethioamide, as a source of sulfide ions. The effects of different synthesis parameters including the type of solvent, temperature, and duration of reactions on the morphology of the CuS and ZnS products were investigated using field emission scanning microscopy and transmission electron microscopy, respectively. The structural aspects of the samples were characterized using powder X‐ray diffraction, Fourier transform infrared spectroscopy, and energy dispersive X‐ray analysis. The optical properties of the samples were studied through their optical absorption and photoluminescence spectra. The photocatalytic ability of the as‐synthesized sulfides was explored by studying the colour removal of methylene blue under ultraviolet light irradiation.