In this study (0-3) P(VDF-TrFE)/BaTiO3 composites containing up to 60 vol% of ceramic phase were prepared by solvent casting or compression molding. Their thermomechanical, dielectric, and piezoelectric properties were investigated, and discussed in the light of the properties of the basic components, the processing route and the resulting morphology. The crystalline structure of the P(VDF-TrFE) matrix was found to be highly dependent on the processing route, while the structure of BaTiO3 was not affected by any of the processing steps. The mechanical properties of the solvent cast materials showed a maximum at 30 vol% BaTiO3, while they increased monotonically with BaTiO3 content for compression molded materials. This difference was attributed to a higher amount of porosity and inhomogeneities in the solvent cast composites. Permittivity as high as 120 and piezoelectric coefficient d(33) up to 32 pC/N were obtained for compression molded composites, and the observed decrease in d(33) with aging time was attributed to the effect of mechanical stress release in the polymer matrix.