Diffusion bonding of V-4Cr-4Ti alloy to pure titanium (Ti) was carried out by hot forging in the temperature range between 1150 • C and 950 • C. The microstructure and mechanical properties of the bonded joint were determined by using light optical microscopy (OM), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), micro-hardness measurements, and shear tests. The results indicate that the sound dissimilar joint can be obtained through hot forging processes. The interface has a width of about 100 µm and can be divided into two distinctive zones: a Widmanstatten structure zone and a β-Ti phase structure zone. According to the micro-hardness distribution profile across the substrates and the interface, the largest hardness of 332 HV was measured in a narrow region between the Ti substrate and the joint, which is remarkably higher than that of the substrates (Ti of 190 HV and V-4Cr-4Ti alloy of 258 HV). The lowest hardness of only 182 HV was found in a region in the V-4Cr-4Ti substrate adjacent to the joint. The shear test showed that the joint has a bonding strength higher than 165 MPa and a fracture of the joint took place in the region with the highest hardness.