An innovative hybrid nanostructure composed of diketopyrrolopyrrole (DPP) oligomers and cadmium sulfide (CdS) nanoparticles was developed to enhance the efficiency of organic– inorganic photovoltaic devices. The DPP-CdS hybrids were synthesized via a solution-phase mixing method, resulting in uniform nanoparticle dispersion along polymer fibrils and strong interfacial coupling. Structural characterization confirmed the coexistence of crystalline CdS domains and partially ordered DPP phases, while spectroscopic analyses indicated notable redshifts and band broadening, evidencing electronic interactions at the interface. The hybrid material displayed significantly broadened light absorption across the 400–700 nm range and an optimized optical bandgap of ~1.92 eV. When implemented in inverted bulk heterojunction solar cells (ITO/PEDOT:PSS/DPP-CdS/PC71BM/Al), the active layer enabled a short-circuit current density of 11.3 mA/cm², open-circuit voltage of 0.82 V, and a power conversion efficiency (PCE) of 5.93%—more than double the PCEs of devices with only DPP (2.61%) or CdS (1.35%). External quantum efficiency exceeded 60% at peak wavelengths, confirming efficient exciton generation a
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