Films of (1-x)Pb(Zn1/3Nb2/3)O3-xPb(Zr0.4Ti0.6)O-3 (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 650degreesC. The root-mean- square surface roughness of a 220 nm thick film was 3 nm as measured by the atomic force microscopy. The 40PZN7 60PZT films annealed at 720degreesC 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 muC/cm(2) and 0.8 V, respectively. The leakage current density was lower than 10(-6)A/cm(2) at an applied voltage of 2.5 V.