A novel sol-gel process suitable for depositing thin-film lead barium titanate has been developed. X-ray diffraction analysis showed perovskite phase crystallization to occur at a temperature as low as 400degreesC with single-phase Pb0.5Ba0.5TiO3 (PBT) resulting at a temperature as low as 500degreesC. Small concentrations of barium carbonate were evident by X-ray diffraction at 400degreesC, and indications of minor, carbonate-containing phases were evident by FTIR at 600degreesC. Deposition of the sol by spin coating on single-crystal and thin-film MgO on silicon resulted in highly oriented PBT films after calcination at 600degreesC. Mixed (100)/(001) films were obtained on single-crystal MgO, whereas entirely (100) films were obtained on thin-film MgO.