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This paper details the enhancement of the optoelectronic properties of Cu-(In, Ga)-Se2 (CIGSe) solar cells through a two-segment process in the ultraviolet (UV)–visible spectral range. These include fine-tuning the DC sputtering power of the absorber layer (ranging from 20 to 40 W at segment I) and thoroughly checking the trace micro-chemistry composition of the absorber layer (CdS, ZnO/CdS, ZnMgO/CdS, and ZnMgO at segment II). After segment I of treatment, the optimal 30 W CIGSe absorber layer (i.e., with a 0.95 CGI ratio) can be obtained, it can be seen that the Cu-rich film exhibits the ability to significantly promote grain growth and can effectively reduce its trap state density. After the segment II process aimed at replacing toxic CdS, the optimal metal alloy (Zn0.9Mg0.1O) composition (buffer layer) achieved the highest conversion efficiency (η) of 8.70%, also emphasizing its role in environmental protection. Especially within the tunable bandgap range (2.48–3.62 eV), the developed overall internal and external quantum efficiency (IQE/EQE) is significantly improved by 13.15% at shorter wavelengths. A photovoltaic (PV) module designed with nine optimal CIGSe cells demonstrated commendable stability. Variation remained within ±5% throughout the 60-day experiment. The PV modules in this study represent a breakthrough benchmark toward a significant advance in the scientific understanding of renewable energy. Furthermore, this research clearly promotes the practical application of PV modules, harmonizes with sustainable goals, and actively contributes to the creation of eco-friendly communities.