Calcium and lanthanum modified lead titanate (PCLT) powder with size in the nanometer range was prepared using a sol-gel technique. PCLT powder annealed at 850°C was incorporated into a polyvinylidene fluoride/trifluoroethylene P(VDF-TrFE) copolymer matrix to form 0.15 mm thick films of 0–3 nanocomposites with ceramic volume fraction (φ) ranging from 0.05 to 0.33. The dielectric and pyroelectric properties of the composites were measured as functions of temperature. The observed permittivity and dielectric loss were found to agree with the predictions of the Bruggeman model. When the ceramic and copolymer phases in these nanocomposites are poled in the same direction, the pyroelectric activities of the two phases reinforce while the piezoelectric activities partially cancel, thereby minimizing the vibration-induced electrical noise in pyroelectric current measurements.