The electrical properties of perovskite-based ferroelectric films were improved by ion modification using rare-earth cations. Thin films of rare-earth-modified lead zirconate titanate [Pb(Zr,Ti)O3] were fabricated on (111)Pt/Ti/SiO2/(100)Si substrates by a chemical solution deposition technique. The substitution of volatile cations in the simple-perovskite oxides, such as Pb2+ in Pb(Zr,Ti)O3 films, enhanced the insulating properties of the film. The crystal anisotropy of the Pb(Zr,Ti)O3 film could be controlled by varying the species and the amount of replacing cations to enhance the spontaneous polarization. Thus, ion modification using Dy3+ cation could enhance the remanent polarization of Pb(Zr,Ti)O3 film consequently.