Composites of pyroelectric ceramics and polymers are very important as their unique features and properties can be easily tailored for various specific applications. Lithium tantalatum oxide (LiTaO3, LT), the pyroelectric ceramic powder has been incorporated into a polyvinylidene fluoride-trifluoroethylene [P(VDF-TrFE) 70/30 mol%] copolymer matrix to form 0-3 composites. The composite films were prepared using 'solvent casting' (SC) method to disperse the ceramic powder homogeneously in the P(VDF-TrFE) copolymer matrix with various wt% of LT powder. In order to derive high pyroelectric performance, the samples were poled. Electric properties, such as the dielectric constant, dielectric loss, and pyroelectric coefficient, have been measured as a function of temperature and frequency. In addition, material figures-of-merit, very important factors for assessing many sensor applications have also been calculated. The results show that the fabricated lead free lithium tantalite: P(VDF-TrFE) composite materials have a good potential for pyroelectric infrared sensor applications.