The paper investigates the effects of Cu particle size on diamond composites experimentally. The hybrid microwave sintering process is proposed to obtain the particle size microstructure throughout the rapid heating. The effects of Cu particles on the hardness, flexural strength, and thermal conductivity are experimentally investigated. The experimental results indicate that the Cu particle size has a significant impact on the physical and mechanical properties of the CuSnFeNi/diamond composites. The smaller the Cu particle size, the larger thermal conductivity, the hardness, and flexural strength are obtained. This study provides an effective means to enhance the mechanical properties of the CuSnFeNi/diamond composite by adjusting the Cu particle size.