This study presents an exhaustive exploration into the development and rigorous evaluation of nano-TiO2-modified recycled aggregates (NT@RAs) as an environmentally sustainable substitute for natural aggregates in concrete applications. A methodical framework was devised for the synthesis and thorough characterization of NT@RAs, emphasizing the optimization of nano-TiO2 loading onto the RA surface and within its intricate porous structure. The investigation encompassed three distinct types of recycled aggregates: recycled glass sands (RGSs), recycled clay brick sands (RCBSs), and recycled concrete sands (RCSs). Of particular interest, NT@RGS, with its properties of an inherently smooth surface texture and low water absorption, was found to exert a favorable influence on the rheological behavior of concrete, manifested in reduced yield stress, thereby underscoring the potential for fine-tuning mix designs to enhance workability. As the substitution levels of NT@RGS and NT@RCBS escalated, an initial decrement in compressive strength was discernible, which subsequently reversed to strength restoration at optimized substitution ratios. This phenomenon is attributed to the synergistic interplay among NT@RA components. Remarkably, NT@RA-incorporated concrete demonstrated unparalleled self-cleaning abilities, surpassing the performance of concrete with direct nano-TiO2 powder incorporation. This comprehensive research contributes significantly to the advancement in sustainable, high-performance photocatalytic construction materials within the realm of concrete technology. It underscores the potential for enhancing not only the rheological and mechanical properties but also the environmental responsiveness of concrete through the innovative utilization of NT@RAs.