Piezoelectric nanocomposites consisting of a polymer matrix and ceramic fillers are candidate components of flexible, wearable, and self-powered electronic devices. The physical discrepancy between ferroelectric polymers and ceramics in a piezoelectric interface makes it difficult to assemble efficient hybrid piezoelectric nano-composites without polarization and extraneous artifacts. Here, we describe the effect of a relaxor ferroelectric terpolymer matrix on the piezoelectric output, which can enhance the energy harvesting or sensor performance of piezoelectric composite device of nanocomposite generators with filler nanoparticles of lead zirconium tita-nate. The dielectric property and reduced ferroelectric hindrance of the proposed terpolymer matrix provides more poling to align the polarization of piezoelectric ceramic fillers compared with a normal ferroelectric copolymer matrix. Therefore, relaxor ferroelectric polymers can be better than normal ferroelectric polymers as the matrix of hybrid polymer-ceramic piezoelectric nanocomposite. This research provides important physical information about the interface between a polymer matrix and ceramic fillers in flexible piezoelectric nano-composite applications.