Spark plasma sintering (SPS) is an effective technique for studying the diffusion bonding of diamond/Cu composites, and has the potential to advance the application of copper matrix composites. This study investigates the SPS diffusion bonding of diamond/Cu composites using a chromium (Cr) interlayer. The effects of process parameters on the microstructure and mechanical properties of the bonding interface were evaluated through shear strength testing and SEM analysis. The results show that shear strength increases with interlayer thickness up to a certain point, after which it decreases. As the bonding temperature, holding time, and bonding pressure increase, defects such as cracks and voids at the diffusion-bonded interface are reduced, resulting in improved shear strength. Under suitable conditions (10 μm interlayer, 810 °C, 60 min, and 10 MPa), the bonding interface is defect-free, achieving a maximum shear strength of 139.89 MPa and a thermal conductivity (TC) of 700.97 W/(m·K), indicating high-quality diffusion bonding.