In this research work, a material system formed of cadmium sulfide combined with chromium atoms was developed to evaluate the influence of chromium concentration on the optical, electrical, structural, and morphological properties of a precursor layer of CdS. It is possible to observe that the transmission spectra increased for all chromium concentrations analyzed. From X-ray diffractograms, we conclude more accurately that CdS presents a mixture of phases, including orthorhombic, hexagonal, and cubic. Furthermore, the impact of adding chromium results in variations in the intensity of two major peaks in the diffractograms and an anomalous shift in the CdS pattern. The calculated resistivities show an invariable behavior of 4.5 × 10 6 Ω cm. In addition, the bandgap values remain practically constant, with values of approximately 2.43−2.44 eV. The addition of chromium at different concentrations leads to surface morphology changes, as observed in SEM images.