We have formed PbTiO3thin films on (100) SrTiO3substrates at a temperature of 350 °C using an ArF excimer laser ablation technique. Until now, PbTiO3films have not been formed at temperatures lower than 500 °C using other thin‐film techniques. The important points in the present study are the laser excitation of the substrate during the film growth and the lattice matching between the film and the substrate. The film deposited on the SrTiO3substrate shows preferential orientation of thec‐axis perpendicular to the substrate surface.