Ferroelectric Pb(Zr0.6Ti0.4)O3 (PZT(60/40)) powder was prepared by a sol-gel method and PZT thick films were fabricated by the screen-printing method on the alumina substrates. The Pt bottom electrodes were screen-printed on the alumina substrate. The PZT(60/40) thick films were annealed at 1050°C for 10min in PbO atmosphere. Pb(Zr0.4Ti0.6)O3 (PZT(40/60)) precursor solution, which prepared by sol-gel method, was spin-coated on the PZT thick films to obtain a densification. These PZT multilayered thick films were annealed at 650°C for 2 h in PbO atmosphere. The upper electrodes were fabricated by screen printing the Ag paste and then firing at 590°C for 10min. Its structural and electrical properties of the PZT thick films with the treatment of PZT(40/60) precursor solution coating were investigated. The coating and drying procedure was repeated 4 times. And then the PZT(40/60) precursor solution was spin-coated on the multilayered thick films. A concentration of a coating solution was 1.5 mol/L and the number of coating was repeated from 0~15. The porosity of the thick films was decreased with increasing the number of coatings. All PZT multilayered thick films showed the XRD patterns of typical peroveskite polycrystalline structure. The relative dielectric constant of the PZT-15 (15: number of solution coatings) thick film were 370. And the PZT-15 thick film shows the remanent polarization of 23.5 μC/cm2 and coercive field of 18.0 kV/cm, respectively.