The reliable bonding of W/CuCrZr is facing a great challenge due to their big difference of mechanical properties, especially the mismatch of thermal expansion coefficient. To find out effective ways to enhance the bonding strength of W/CuCrZr, 3 experimental schemes, ie, vacuum diffusion bonding without any interlayer (benchmark scheme), oxygen-free high thermal conductivity (OFHC) copper foil as the interlayer, and diamond/Cu composite as the interlayer are designed and studied in this paper. It is found that OFHC copper foil can effectively reduce the bonding defects and improve the bonding strength. The average tension strength and shear strength of the specimens are approximately 75 and 190MPa, respectively. In addition, it is found that diamond/Cu composite is a good choice for strengthening the bonding by completing vacuum sintering of the composite and its diffusion bonding with W and CuCrZr at the same time. The average tension strength of the samples is around 65MPa, and the average shear strength is approximately 150MPa with the highest one up to 180MPa.