The Pb(Zr1-xTix)O-3 multilayered films consisting of Pb(Zr0.8Ti0.2)O-3 and Pb(Zr0.2Ti0.8)O-3 layers with different orientations were deposited by radio frequency magnetron sputtering with PbOx and LaNiO3 (LNO) buffer layers. The PbOx and LNO buffer layers lead to the (001)/(100) and (101)/(110) orientations of the multilayered films, respectively. The orientation dependence of electrical properties of the multilayered films was investigated. Enhanced remnant polarization (2P(r)=79.3 mu C/cm(2)) and dielectric constant (epsilon(r)=857) were obtained for the multilayered films with (001)/(100) orientation as compared to those of the multilayered films with other orientations. These results reveal that the orientation control is important in obtaining good electrical properties.