Piezoelectric ceramics play an important role in various electronic applications. However, traditional ceramics are difficult to be used in some complicated structures, due to their low flexibility and high brittleness. To solve this problem, this study prepared and investigated ceramic/polymer composites that can utilize a good flexibility of polymers. Polyvinylidene fluoride-trifluoroethylene (PVDF-TrFE) and 0.77(Bi1/2Na1/2)TiO3-0.23SrTiO3 (BNST23) ceramics were selected to fabricate the composites. Ceramic/polymer composites were prepared using various volume fractions of BNST23 ceramics. The distribution of piezoceramic particles in BNST23/PVDF-TrFE composites was investigated using optical microscopy (OM) and scanning electron microscopy (SEM). The dielectric and piezoelectric properties of the composites were significantly influenced by the volume fraction of the piezoelectric ceramics. As a result, the highest piezoelectric constant (d33) of 56 pC/N was obtained in a composites with 70% volume fraction of BNST23 ceramics. Accordingly, it is expected that BNST23/PVDF-TrFE composites can be applied to various sensor applications.