Films of (1− x)Pb(Zn1/3Nb2/3)O3- xPb(Zr0.4Ti0.6)O3 ( x = 0.6, 40 PZN-60PZT) were deposited on Pt/TiO2/SiO2/Si substrate through spin coating. Using a combination of homogeneous precursor solutions and two-step pyrolysis process, it was possible to obtain the 40PZN-60PZT thin films of perovskite phase virtually without pyrochlore phase precipitation after annealing above 650°C. The root-mean-square surface roughness of a 220 nm thick film was 3 nm as measured by the atomic force microscopy. The 40PZN-60PZT films annealed at 720°C showed a well-saturated hysteresis loop at an applied voltage of 5 V with remanent polarization ( P r ) and coercive voltage ( V c ) of 29 μ C/cm2 and 0.8 V, respectively. The leakage current density was lower than 10− 6A/cm2 at an applied voltage of 2.5 V.