Ti and Cu were used as interlayer materials, and the diffusion bonding of Be/CuCrZr alloys were carried out onto Be side by hot isostatic pressing. The four Be samples had different surface roughness. The coating, interface behavior and microstructure of the diffusion bonded alloys were studied by AES, SEM (EDS), room-temperature shear test and XRD. The results show that the Ti coating band (9 μm thickness) and the Cu coating band (35 μm thickness) are homogeneous, and few harmful ingredients are observed. Dual-target and single-side coating technology is favorable to reduce the Ti-coating oxidation. Shearing strength of the Be/CuCrZr interface is increased significantly, with the highest up to 243 MPa. But effect of the different surface roughness on the shearing strength is not obvious. The bonding strength of Be-Ti is high, and all the shear fracture of the samples occurs in the Cu layer.