Lead strontium titanate (PbxSr1-xTiO3) (x=0.3–1.0) ceramic targets were prepared by the conventional powder-processing method. Thin films of these compositions were deposited on platinized silicon substrates by pulsed laser deposition technique. X-ray diffraction studies of the ceramic targets showed that the lattice structure changes from tetragonal to cubic phase with the increase of Sr content in PbTiO3. Raman spectroscopic studies of PbxSr1-xTiO3 (PST) ceramics and thin films showed that the soft mode decreases to lower frequency and finally disappear at around 60–70 at% Sr content, which confirms the tetragonal to cubic phase transition at room temperature. Dielectric constant measured for PST thin films was in the range of 900–1500 at 1 MHz, with maximum value obtained for PST30 thin film. The loss tangents at room temperature were in the range of 0.07–0.1 for PST thin films with different compositions.