Diamond particle-reinforced Zr-alloyed Cu matrix (diamond/Cu-xZr) composites were produced by a gas pressure infiltration route, with x = 0.0, 0.3, 0.5, 0.75, and 1.0 wt.%. The x-ray diffraction, scanning electron microscopy, and transmission electron microscopy characterization confirms the formation of ZrC at the diamond/Cu interface. With increasing Zr content, the tensile, bending, and compressive strengths of the diamond/Cu-Zr composites are found to firstly increase and then decrease. The maximum tensile, bending, and compressive strengths at 0.75 wt.% Zr are 108, 360, and 441 MPa, respectively. The variation of the mechanical properties is attributed to the formation of interfacial ZrC. The increase in amount of ZrC strengthens the interface, but large ZrC particles formed at high Zr content are harmful to the interfacial bonding. The result suggests that the mechanical properties of diamond/Cu composites can be enhanced by Cu matrix alloying with Zr.