Heterolayered K(Ta,Nb)O3/Pb(Zr,Ti)O3 thin films on Pt/Ti/SiO2/Si substrates were prepared by a sol-gel process and spin-coating method. The structural and electrical properties were measured to investigate the possibility of application as an electrocaloric effect device. All specimens exhibited dense and uniform cross-sectional structures without pores, and the average thickness of the specimen coated six times was approximately 394 nm. Curie temperatures were observed at 5℃ or less in type-Ⅰ and 10℃ in type-Ⅱ specimens, respectively. Type-Ⅱ specimens coated 6 times showed a relative dielectric constant of 758 and remanent polarization of 9.71 μC/cm2 at room temperature. The maximum electrocaloric effect occurred between 20 and 25℃, slightly higher than their Curie temperature, and the electrocaloric property (ΔT) of the type-Ⅱ specimens coated 6 times was approximately 1.2℃ at room temperature.