Triboelectric nanogenerators (TENGs) offer a promising approach for mechanical energy harvesting, but an effective strategy for enhancing the output performance is a crucial requirement. Though many studies have been performed to maximize the triboelectrification phenomenon on the surface of dielectric materials, studies for improving electrostatic induction phenomenon inside the dielectric materials have not yet been conducted. Here, we propose a high output performance TENG with a composite of butylated melamine formaldehyde (BMF) matrix and the high dielectric constant particles of CaCu3Ti4O12 (CCTO) as an excellent dielectric layer for enhancing the electrostatic induction phenomenon. The high dielectric constant CCTO particles result into a strong polarization of the dielectric materials under the triboelectric field. As a consequence, the charge induction in the bottom electrode is enhanced thereby increasing the triboelectric output power. A rotation-type freestanding mode TENG based on BMF-CCTO 1wt% composite has produced an RMS voltage and a current density (268 V and 25.8 mA/m2) which is about 3 times higher than that (113.2 V and 8.7 mA/m2) of the TENG based on pure BMF. The strategy of incorporating the high dielectric constant CCTO particles is completely general and can be applied to any polymer matrix in order to enhance the output performance of TENGs.