Thin films of BaTiO3 and PZT (lead zirconate titanate, 47%PbTiO3, 53%PbZrO3) have been produced by laser irradiation of the appropriate ceramic targets and deposition of the ejected and vaporized material on planar substrates. The microstructural changes during thermal processing of these films have been studied by scanning electron microscopy/energy dispersive x-ray spectrometry (SEM/EDX), transmission electron microscopy (TEM), differential scanning calorimetry (DSC), x-ray diffraction (XRD), and by measurement of electrical properties. Films have been deposited using both Nd/YAG and excimer lasers and on unheated as well as heated substrates. Excimer films are considerably smoother than the Nd/YAG films, and the uniformity of the as-deposited microstructures is promoted by substrate heating. However, ferroelectric hysteresis loops were only observed for the considerably less smooth Nd/YAG PZT films; thermal treatment did little to improve the smoothness of these films. An excimer BaTiO3 film deposited on a heated substrate showed crystallographic alignment and had a dielectric constant of −100. Efforts are underway to combine the best features of films produced by both methods.