The electron cyclotron resonance plasma enhanced chemical vapor deposition (ECR PECVD) method is used to prepare ferroelectric PbTiO3 films. Single-phase perovskite PbTiO3 films with smooth surfaces and fine grain size were successfully fabricated on Pt/Ti/SiO2/Si substrates at low temperatures of 400–500 °C using metal-organic (MO) sources. The chemical compositions, structural phases, surface morphologies, and depth profiles of the PbTiO3 thin films were investigated using EDS, XRD, SEM, RBS, and AES. Variations of those properties with process temperature and gas supply ratio are discussed. When the process temperature was above 450 °C, the stoichiometric perovskite PbTiO3 films could be obtained even though the MO source supply ratio was varied in a wide range if the oxygen supply was sufficient.