CdS:Al thin films were fabricated on a glass substrate using the CBD method. The effect of aluminum incorporation on the structural, morphological, vibrational, and optical properties of CdS thin layers was investigated by X-ray diffraction (XRD), Raman spectroscopy (RS), atomic force microscopy (AFM), scanning electron microscopy (SEM), and UV-visible (UV-vis) and photoluminescence (PL) spectroscopies. XRD analysis of deposited thin films confirmed a hexagonal structure with a preferred (002) orientation in all samples. The crystallite size and surface morphology of the films are modified with aluminum content. Raman spectra exhibit fundamental longitudinal optical (LO) vibrational modes and their overtones. Optical properties were studied for each thin film. Here, it was observed that the optical properties of thin films are affected by the incorporation of aluminum into the CdS structure.