The conversion of atmospheric CO₂ into valuable fuels while simultaneously storing renewable energy represents a grand challenge in sustainable energy research. Here, we report the design and fabrication of ultrafast photo-electrocatalytic nanoparticle networks engineered for dual CO₂ reduction and high-energy storage within hybrid quantum materials. The system integrates plasmonic nanoparticles with quantum dots and 2D conductive frameworks, establishing a synergistic interface for rapid charge separation and transfer. Under simulated solar illumination, the networks achieve femtosecond-scale electron mobility, driving selective CO₂ reduction to methanol while concurrently storing charge in quantum-confined domains. This hybrid design bridges photonic excitation and electrochemical storage mechanisms through quantum coupling effects, yielding unprecedented energy densities (up to 420 Wh kg⁻¹) and Faradaic efficiencies above 93%. Structural and spectroscopic analyses confirm robust electron delocalization across multi-phase junctions, stabilizing catalytic intermediates and preventing recombination losses. These findings reveal a new materials platform capable of simultaneous carbon valorization and renewable energy storage, representing a transformative step toward closed-loop, carbon-neutral energy systems.