In the present work, we utilized Cu-Co@TiO2 NCs (as a substitute of Fe+2 in UV/PMS/ Fe+2 system) for the degradation of model dyes such as Chicago Sky Blue 6B (CSB-6B) and Acid Yellow 17 (AY-17). The Cu-Co@TiO2 NCs synthesized via a simple reduction method by using NaBH4 as a reducing agent. The as-prepared NCs are characterized by SEM, EDX, FTIR, and XRD. The degradation through the UV/PMS/Fe+2 system is reported to be 62% and 59% (at optimized conditions) for CSB-6B and AY-17, respectively. Whereas the degradation by UV/PMS/ Cu-Co@TiO2 NCs system at optimized conditions is 98% and 97% for CSB-6B and AY-17, respectively. The Cu-Co@TiO2 NCs are found to remain stable in the photocatalytic dye degradation reaction carried out by the UV/PMS/ Cu-Co@TiO2 NCs system. The Co@TiO2 NCs therefore can be used repeatedly in UV/PMS/ Cu-Co@TiO2 NCs systems for their promising applications in wastewater treatment.