In this study, cadmium Sulfide (CdS) thin films were synthesized on quartz substrates using an infrared pulsed laser deposition (IR-PLD) technique under high vacuum (~10−6 Torr) conditions. X-ray diffraction was used to evaluate the structural features. According to X-ray analysis, the deposited CdS films are crystalline and have a favored orientation on a plane (110) of an orthorhombic. The peak intensity and the average crystallite size increases with increasing the film thickness. After annealing at 300 °C, the orthorhombic phase transformed into a predominant hexagonal phase and the same result was obtained by SEM photographs as well. Spectrophotometric measurements of transmittance and reflectance of the CdS films were used to derive optical constants (n, k, and absorption coefficient α). The optical band gap energy was found to be 2.44 eV. The plasma plume formation and expansion during the film deposition have also been discussed. The photocurrent response as a function of the incident photon energy E (eV) at different bias voltages for different samples of thicknesses (85, 180, 220 and 340 nm) have been studied, indicating that the photocurrent increases by increasing both the film thickness and photon energy with a peak in the vicinity of the band edge. Thus, the prepared CdS films are promising for application in optoelectronic field.