With the ever increasing requirements for the structural health monitoring systems, the deposition of the piezoelectric films on the metallic or structural materials has turned out to be an important issue. Pb(Mg, Nb)O3-PbTiO3 films with different buffer layers, i.e., in situ NiO, pre-fabricated NiO and LaNiO3, were successfully deposited on the Ni foil via the chemical solution deposition. The crystal structures and electric performances showed evident dependence on the buffer layer. Pre-deposited NiO and LaNiO3 efficiently prevented the diffusion and complex reactions occurring at the interface, offered abundant nucleation sites, and thus helped the formation of pure high-qualified perovskite PMN-PT films at higher annealing temperatures.