Effects of the lead zinc niobate (PZN) addition and postannealing temperature on the electrical properties of the lead zirconate titanate (PZT) films were observed to improve electrical properties of the PZT film. The PZN content was varied from 0% to 40%, and the postannealing temperature was varied from 500to900°C. The as-deposited film had a fairly dense microstructure without any cracking and showed a single perovskite phase formed with nanosized grains. Meanwhile, rapid grain growth was observed when the postannealing temperature was increased from 700to900°C. The PZN-added PZT film showed poorer electrical properties than the pure PZT film did when the films were annealed at 700°C but higher remnant polarization, dielectric constant, and piezoelectric response when the films were annealed at 900°C. Remnant polarization value, relative dielectric constant, and piezoelectric constant of the 20% PZN-added PZT films annealed at 900°C were 50.0μC∕cm2, 1643, and 200pC∕N, respectively, which are values sufficiently high to be comparable with the bulk specimen sintered at 1200°C.