The effects of the dielectric constant of the powder phase on lead zirconate titanate (PZT)/PZT sol-gel composite films were investigated to tailor their electrical properties. Three types of PZT powders were used to fabricate three different PZT/PZT sol-gel composite films. The PZT powders had the same electromechanical coupling coefficient but different relative dielectric constants. The PZT/PZT films were fabricated on a 3 mm-thick titanium substrate using an automatic spray coating system, and their properties were investigated. The relative dielectric constants of the PZT/PZT films were successfully controlled by tailoring the properties of the PZT powder phase. However, the piezoelectric constants showed a tendency different to those of the raw powders, because of the poor poling degree. This was overcome by conducting poling at a high temperature.