Using the same conditions and various starting materials, such as lead acetate trihydrate, tetrabulyl titanate, zirconium n-butoxide, and acetylacetone, two kinds of solid precursors, lead zirconate titanate (PZT, Zr/Ti=15/85) and lead titanate (PT), were fabricated. With three different combinations, namely, PZT, PT/PZT-PZT/PT, and PT/PZT/-/PZT/PT, three multilayer thin films were deposited on three Pt-Ti-Si3N4-SiO2-Si substrates by a modified sol-gel process. The fabrication process of the thin films is discussed in detail. We found that there is a large built-in stress in the thin film, which can be diminished by annealing at 600 ℃, when the gel is turned into solid material through drying and sintering. The Raman scattering spectra of the films with different compositions and structures were investigated. With the help of X-ray diffraction (XRD) analyzer and Raman scattering spectra analyzer, it was found that the thin films with the PT/PZT-PZT/PT structure have reasonable crystallinity and less residual stress. XRD testing shows that the diffraction pattern of the multilayer film results from the superimposition of the PZT and PT patterns. This leads to the conclusion that the PT/PZT-PZT/PT multilayer thin film has a promising future in pyroelectric infrared detectors with high performance.