In the present investigation, an easy approach for the synthesis of nanostructures composed of carbon spheres (CSs) and ZnS was demonstrated. CSs were prepared by aerosol-assisted chemical vapor deposition of toluene at 1050 °C and were characterized by different techniques, including X-ray diffraction, Raman spectroscopy, scanning electron microscopy, transmission electron microscopy, and thermogravimetric analysis. Further, their composite with ZnS nanoparticles (NPs) was synthesized by using solvothermal decomposition of a single-source precursor in the presence of ethylene glycol. The competence of the resultant composite material was tested in the photodegradation of eriochrome black-T and methylene blue, and the results were compared with those obtained for the bare ZnS NPs. The substantial increase in the photodegradation efficiency of the composite is attributed to the large surface area provided by the CSs to the ZnS NPs for dye reduction.