Ferroelectric PbTiO3films were deposited by ion‐beam‐assisted deposition (O2+Ar 75–150 eV). The effects of ion bombardment on the Pb/Ti ratio and the structures of the film are discussed. For a given target‐substrate distance and substrate temperature, the Pb/Ti ratio decreased with increasing bombarding beam energy. Compared with the films deposited without ion bombardment, the deposition rate was increased under ion bombardment, which is attributed to an increase in the surface reaction rate. The crystal grains are larger for films deposited under ion bombardment, which implies that ion bombardment enhances the surface mobility of adatoms and hence the growth kinetics of the growing films. Dielectric and ferroelectric properties of the as‐deposited films are also reported.