The coating solutions of nanostructured (Pb 1-x Sr x )TiO 3 (PST) thin films have been prepared by the sol-gel combined metallo-organic decomposition method. The coating solutions were deposited on Pt/Ti/SiO 2 /Si substrates using a spin-coating technique with spinning speed of 4300 rpm and annealed at 650 C. The effect of Sr content in reducing the grain size and tetragonal distortion of PST films has been studied. The optimum conditions for crystalline phase formation in the films have been analyzed by thermogravimetric, differential thermal analysis and Fourier transform infrared spectroscopy. The phase and microstructure of the films were studied by X-ray diffraction (XRD) and atomic force microscopy (AFM). The XRD pattern shows that the PST thin films are crystallized into tetragonal structures without any impurity phase and the distortion ratio reduces with increasing Sr concentration. The AFM results indicate an increase in grain size with increasing annealing temperature of the film and reduction in grain size with increasing Sr concentration.