CdS thin films were grown on an FTO substrate at different temperatures, employing the low-cost hydrothermal method. All the fabricated CdS thin films were studied using XRD, Raman spectroscopy, SEM, PL spectroscopy, a UV–Vis spectrophotometer, photocurrent, Electrochemical Impedance Spectroscopy (EIS), and Mott–Schottky measurements. According to the XRD results, all the CdS thin films were formed in a cubic (zinc blende) structure with a favorable (111) orientation at various temperatures. The Scherrer equation was used to determine the crystal size of the CdS thin films, which varied from 25 to 40 nm. The SEM results indicated that the morphology of thin films seems to be dense, uniform, and tightly attached to the substrates. PL measurements showed the typical green and red emission peaks of CdS films at 520 nm and 705 nm, and these are attributable to free-carrier recombination and sulfur vacancies or cadmium vacancies, respectively. The optical absorption edge of the thin films was positioned between 500 and 517 nm which related to the CdS band gap. For the fabricated thin films, the estimated Eg was found to be between 2.50 and 2.39 eV. According to the photocurrent measurements, the CdS thin films grown were n-type semiconductors. As indicated by EIS, resistivity to charge transfer (RCT) decreased with temperature, reaching its lowest level at 250 °C. Flat band potential and donor density were found to fluctuate with temperature, from 0.39 to 0.76 V and 4.41 × 1018to 15.86 × 1018cm−3, respectively, according to Mott–Schottky measurements. Our results indicate that CdS thin films are promising candidates for optoelectronic applications.