Pb(Zr,Ti)O 3 thin films (Pb:Zr:Ti=1:0.52:0.48) were prepared on various single-crystal substrates via dipping-pyrolysis process by use of metal naphthenates as starting materials. The alignments of these films were examined by X-ray diffraction (XRD) θ–2 θ scans and β scans (pole figures). The films grown on Nb-doped SrTiO 3, MgO or LaAlO 3 showed an epitaxial relationship with substrates after heat treatment at 750°C, while those grown on sapphire and Si wafers exhibited polycrystalline or amorphous characteristics. Epitaxial films on SrTiO 3 and LaAlO 3 were found to consist of a c-axis oriented tetragonal phase, to minimize the lattice misfit with the substrates. These epitaxial films exhibited very smooth surfaces by SEM and AFM observations. In addition, the fluctuation of in-plane alignment was significantly dependent on the lattice-misfit values.