Well-crystallized polycrystalline films of tetragonal PbTiO3 have been synthesized on Ti metal substrates in concentrated alkaline solutions of Pb(OH)2 containing KOH by the hydrothermal method under saturated vapor pressure (2.0 MPa) at 200 °C. The film microstructure depended strongly on the Pb(OH)2 and KOH concentration. The grain size became larger from approximately 0.6 to 6 μm with an increase of KOH concentration from 1 to 4 M at 0.07 M Pb(OH)2, whereas the grains decreased in size with an increase of Pb(OH)2 concentration at 1 M KOH concentration. PbTiO3 film prepared in the aqueous solution of 0.07 M Pb(OH)2 containing 2 M KOH showed a relative dielectric constant of about 215 and loss of about 5% at 1 kHz.