ZnS-ZnO nanocomposites (NCs) were successfully synthesized via thermal treatment of as-synthesized ZnS nanostructured spheres (NSs). By applying multiple characterization technology, such as XRD, FESEM, EDS and UV-Vis, the obtained samples were fully characterized. After modification, the light-absorption performance of ZnS NSs to visible light was significantly enhanced. The band gap of ZnS-ZnO NCs was estimated to be 2.7 eV. The photocatalytic test indicated that ZnS-ZnO NCs exhibited enhanced photocatalytic activity in contrast to the pristine ZnS due to the effective charge separation. A photocatalytic mechanism was proposed to illustrate the photocatalytic reduction process. The formation mechanism of ZnS NSs and ZnS-ZnO NCs was also proposed in detail.