Understanding of the triboelectric charge accumulation from the view of materials plays a critical role in enhancing the output performance of triboelectric nanogenerator (TENG). In this paper, we have designed a feasible approach to modify the tribo-material of TENG by filling it with high permittivity nanoparticles and forming pores. The influence of dielectricity and porosity on the output performance is discussed experimentally and theoretically, which indicates that both the surface charge density and the charge transfer quantity have a close relationship with the relative permittivity and porosity of the tribo-material. A high output performance TENG based on a composite sponge PDMS film (CS-TENG) is fabricated by optimizing both the dielectric properties and the porosity of the tribo-material. With the combination of the enhancement of permittivity and production of pores in the PDMS film, the charge density of ∼19 nC cm(-2), open-circuit voltage of 338 V, and power density of 6.47 W m(-2) are obtained at working frequency of 2.5 Hz with the optimized film consisting of 10% SrTiO3 nanoparticles (∼100 nm in size) and 15% pores in volume, which gives over 5-fold power enhancement compared with the nanogenerator based on the pure PDMS film. This work gives a better understanding of the triboelectricity produced by the TENG from the view of materials and provides a new and effective way to enhance the performance of TENG from the material itself, not just its surface modification.