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Cu-0.4Cr (wt.%) alloys with the microalloying of Hf elements were subjected to a modified rolling–aging process to achieve high strength, high electrical conductivity and high ductility simultaneously. Transmission electron microscopy and X-ray line broadening analysis were conducted to characterize the microstructures of these alloys. Deformation twins and high-density dislocations were introduced into the copper alloys via the modified rolling–aging process and the microalloying of Hf, improving the mechanical properties of copper alloys. The Cu-Cr-Hf alloy with a reduced Hf content performed well in terms of strength, electrical conductivity and ductility. The microalloying of 0.4 wt.% Hf in the Cu-0.4Cr alloy was sufficient to achieve a good combination of high tensile strength (593 MPa), high uniform elongation (~5%) and high electrical conductivity (80.51% IACS).