Ordered mesoporous Cd(x)Zn(1-x)S ternary compound semiconductors were prepared with a simple nano-casting method using 3-D cubic Ia3d meso-structured silica, KIT-6, as a hard-template with the easily available precursors of 3CdSO4 x 8H2O and ZnSO4 x 7H2O. Thermal reduction of impregnated precursors resulted in the crystalline networks within the mesopore of the silica template, then the ordered mesoporous Cd(x)Zn(1-x)S materials were obtained by etching the silica template with NaOH aqueous solution. The synthesized Cd(x)Zn(1-x)S materials exhibit high surface area, uniform pore size, single gyroidal tetragonal I41/a meso-structure, crystalline framework, and finely tuned band gap energies by controlled chemical composition.