This study presents a forward-leaning approach to constructing hybrid organic–inorganic nanomaterials through a photoelectrocatalytic pathway tailored for sustainable energy generation and selective CO₂ conversion. The work integrates light-driven charge activation with surface-engineered catalytic interfaces, allowing the material to operate under mild conditions while maintaining high stability. By combining organic donor groups with inorganic semiconductor frameworks, the system ensures efficient charge mobility, stronger adsorption of CO₂, and controlled intermediate formation. This synergy enables faster reaction kinetics and enhances product selectivity without relying on harsh chemical inputs. Experimental results show that the hybrid structures exhibit notable improvements in photocurrent density, quantum efficiency, and carbon-based product yield when compared with conventional single-phase catalysts. The material’s architecture also supports extended operational durability, mitigating surface deactivation and maintaining consistent performance across repeated cycles. Mechanistic analysis indicates that the coexistence of organic functionalities and inorganic lattice sites opens new reaction channels, creating a balanced environment for electron transfer and catalytic turnover. This approach demonstrates a practical and scalable route toward low-energy CO₂ transformation technologies, offering a blueprint for advancing renewable-driven chemical production. The findings underscore the potential of photoelectrocatalytic hybrid materials as versatile platforms capable of bridging energy conversion and carbon-management applications. The study ultimately lays a clear foundation for next-generation catalysts engineered to operate at the crossroads of sustainability, efficiency, and molecular precision.