In this study, we aimed to improve our understanding of the response mechanisms associated with the formation of CdS thin films. CdS thin film remains the most valuable option for many researchers, since it has shown to be an effective buffer material for film-based polycrystalline solar cells (CdTe, CIGSe, CZTS). We performed experimental and numerical simulations to investigate the effect of different thiourea concentrations on the characteristics of the CdS buffer layer. The experimental results reveal that an increase in thiourea concentrations had a direct effect on the optical results, with bandgap values ranging from (2.32 to 2.43) eV. XRD analysis confirmed that all deposited films were polycrystalline, except for [1/0.75], where there is no CdS formation. Electrical studies indicated that CdS with a molar ratio of [Cd]/[S] of 1 had the maximum carrier concentration (3.21 × 10¹⁴ cm⁻³) and lowest resistivity (1843.9 Ω·cm). Based on the proposed mechanism, three kinds of mechanisms are involved in the formation of CdS layers. Among them, the ion-by-ion mechanism has a significant effect on the formation of CdS films. Besides, modelling studies reveal that the optic-electrical properties of the buffer layer play a crucial role in influencing the performance of a CIGS solar cell.