The microstructures of sputtered thin films of lead-lanthanum zirconate-titanate (PLZT) on (0001) sapphire substrate have been studied using scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Thin films of polycrystalline PLZT (9/65/35), Pb0.91La0.09Zr0.65Ti0.35O3, were prepared on a (0001) sapphire substrate by reactive sputtering, using the dc-magnetron system with a multitarget, Pb, La, Zr, and Ti at the substrate temperature of 700 °C. The PLZT thin films comprised (111) oriented small crystallites of PLZT. Although the average direction of the crystal orientation corresponded to the ideal epitaxial relationship (111) PLZT ‖ (0001) sapphire, the individual crystallites showed misalignment in both the growth direction and the film plane. The thin films could not be considered epitaxially grown films. From analysis of the TEM images, there exists an interfacial region between the PLZT thin film and the substrate. The interfacial region comprises ordered clusters of (111), disordered (101), and/or (110) PLZT crystallites. The presence of the interfacial region will suppress ideal epitaxial growth with uniform crystal orientation. It is confirmed that the addition of the buffer layer of graded composition of PLT-PLZT, between the substrate and the PLZT thin film, will suppress the formation of the disordered interfacial region and will enhance the epitaxial growth of the (111) PLZT on (0001) sapphire with three-dimensional crystal orientations.