We have demonstrated a template-free large-scale synthesis of nanostructured Cd(x)Zn(1-x)S by a simple and a low-temperature solid-state method. Cadmium oxide, zinc oxide, and thiourea in various concentration ratios are homogenized at moderate temperature to obtain nanostructured Cd(x)Zn(1-x)S. We have also demonstrated that phase purity of the sample can be controlled with a simple adjustment of the amount of Zn content and nanocrystalline Cd(x)Zn(1-x)S(x = 0.5 and 0.9) of the hexagonal phase with 6-8 nm sized and 4-5 nm sized Cd(0.1)Zn(0.9)S of cubic phase can be easily obtained using this simple approach. UV-vis and PL spectrum indicate that the optical properties of as synthesized nanostructures can also be modulated by tuning their compositions. Considering the band gap of the nanostructured Cd(x)Zn(1-x)S well within the visible region, the photocatalytic activity for H2 generation using H2S and methylene blue dye degradation is performed under visible-light irradiation. The maximum H2 evolution of 8320 μmol h(-1)g(-1) is obtained using nanostructured Cd(0.1)Zn(0.9)S, which is four times higher than that of bulk CdS (2020 μmol h(-1) g(-1)) and the reported nanostructured CdS (5890 μmol h(-1)g(-1)). As synthesized Cd(0.9)Zn(0.1)S shows 2-fold enhancement in degradation of methylene blue as compared to the bulk CdS. It is noteworthy that the synthesis method adapted provides an easy, inexpensive, and pollution-free way to synthesize very tiny nanoparticles of Cd(x)Zn(1-x)S with a tunnable band structure on a large scale, which is quite difficult to obtain by other methods. More significantly, environmental benign enhanced H2 production from hazardous H2S using Cd(x)Zn(1-x)S is demonstrated for the first time.