Cd 1−x Zn x S thin films of variable compositions (x = 0.2, 0.4, 0.6, 0.8) were deposited on glass at room temperature by thermal evaporation process. The prepared samples were annealed at two different temperatures (300°C, 400°C) for 1 hour in ambient air. The effects of post-annealing on the structural and optical characteristics were investigated using X-ray diffraction (XRD), spectrophotometry, and Raman spectroscopy (RS) methods. XRD studies suggested that the annealed and as-deposited samples belong to wurtzite structure for all Zn concentrations with a preferential orientation along (002) plane. Spectrophotometry analysis of the samples revealed that the energy band gap decreased with annealing temperature. RS investigated different phonon bands and crystalline phases. Two longitudinal optical phonon modes (1-LO, 2-LO) corresponding to monophase hexagonal structure were observed for all Cd 1−x Zn x S samples. The observed red-shift and anti-symmetrical nature of the 1-LO phonon mode can be associated with annealing, while the overall blue-shift, except for x 0.6, was caused by the structural disorders in periodic Cd atomic sub-lattices and broken translational symmetry. The spectroscopic results were strengthened by the XRD studies and their results are consistent.