The (SnO2+CNTs/SnS) thin films deposited by the spray pyrolysis technique were used as photocatalytic application. The changes of structure, topography and optical characteristics upon the deposition of the upper layer were studied. The XRD revealed poly-crystalline mixed Orthorhombic and Zincblende phases and SnO 2 and C phases following the deposition of the upper layer. The FE-SEM images suggest the homogenous porous structure and the large differences in the surface morphology following the deposition of the upper layer. The UV-visible absorbance was enhanced, and the optical bandgap variation to tune to the peak of the solar spectrum. As the pH value rose beyond 8, the photocatalytic activity rose. The efficiency of degradation increased with deposition of the upper layer with the value rising to 95.84% after exposure to 120 min of solar radiation. These results lead to another approach to adjust the structural and optical quality of the SnS thin film by a simple method of nano-heterojunctions with an upper layer to apply to photocatalysis.