Ferroelectric PbTiO3 thin films of various surface morphologies (dense or highly porous) were prepared on Si(111) and Pt/ Ti/Si(111) substrates by electrostatic spray deposition (ESD). Substrate temperature was the key factor affecting the film morphology, and the appropriate substrate temperature was a little higher than the boiling point of the solvent in precursor. The PbTiO3 films prepared by repeated deposition/pyrolysis cycles were porous due to the preferential deposition of charged droplets. Modified ESD was developed to densify the porous films by repairing the cracks and pores in the porous films. The dielectric constant and the dissipation factor of the PbTiO3 film at 100 kHz were 177 and 0.025, respectively. A model was proposed to illustrate the deposition process of the films. (C) 2003 Elsevier B.V. All rights reserved.