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The pursuit of an advanced functional coating that simultaneously combines high hardness, wear resistance, and superior electrical conductivity has remained an elusive goal in the field of copper alloy surface enhancement. Traditional solid solution alloying methods often lead to a significant increase in electron scattering, resulting in a notable reduction in electrical conductivity, making it challenging to achieve a balance between high hardness, wear resistance, and high conductivity. The key lies in identifying a suitable microstructure where dislocation motion is effectively hindered while minimizing the scattering of conductive electrons. In this study, a novel Cu-MoSi2 coating was successfully fabricated on a CuCrZr alloy surface using the coaxial powder feeding high-speed laser cladding technique, with the addition of 10–30% MoSi2 particles. The coating significantly enhances the hardness and wear resistance of the copper substrate while maintaining favorable electrical conductivity. As the quantity of MoSi2 particles increases, the coating's hardness and wear resistance gradually improve, with minimal variance in conductivity. Among the coatings, the Cu-30%MoSi2 coating stands out with the highest hardness (974.5 HV0.5) and the lowest wear amount (0.062 mg/km), approximately 15 times the hardness of the copper base material (65 HV0.5) and only 0.45% of the wear amount (13.71 mg/km). Additionally, the coating exhibits a resistivity of 0.173 × 10−6 Ω·m. The extraordinary hardness and wear resistance of these coatings can be attributed to the dispersion strengthening effect of MoxSiy particles, while the high electrical conductivity is due to the low silicon content dissolved into the copper from the released MoSi2 particles, as well as the rapid cooling rates associated with the high-speed laser cladding process. [ABSTRACT FROM AUTHOR]