Studies on strontium-doped lead zirconate titanate (PSZT) have been reported for its high piezoelectric and ferroelectric properties. For PSZT to exhibit pronounced piezoelectric behaviour it must have a crystalline grain structure (perovskite orientation). This paper is a study of the deposition of PSZT thin films by RF magnetron sputtering and the effect of cooling rate, after deposition at temperatures between 500 °C and 700 °C. X-Ray Diffraction (XRD) results are used to show how a cooling rate of 5 °C/min increases the degree of perovskite orientation in sputtered films, when compared to a cooling rate of 15 °C/min. The absence of significant shifts in the positions of diffraction peak patterns in XRD results are used to demonstrate low stress in the deposited films. Atomic Force Microscope (AFM) imaging is used to show the crystalline nature of the PSZT thin films.