Dielectric materials, commonly referred to as electrical insulators, have received much attention owing to their strong electron bonding, good support of electric fields, and low energy loss. In particular, polarization and depolarization that occur in dielectrics as a result of an external electric field has been investigated as a means to efficiently charge and discharge electricity, which are very useful when applied to capacitors. Dielectrics have also been widely used as charge accepting materials in triboelectric nanogenerator (TENG). So far, various dielectric materials such as polydimethylsiloxane (PDMS), poly(methyl methacrylate) (PMMA), polyimide (PI), polyvinylidene fluoride (PVDF), and polytetrafluoroethylene (PTFE) have been used without any modifications and the electrical signals were not enough. Very recently, the modification of properties such as compressibility surface potential, and hydrophobicity in a few TENGs has been reported, however, most of them have focused on partial reports on the effects of the output performance. Here, we present rational design of effective polymer dielectrics for high-output triboelectric nanogenerator based on PDMS, PI, and PVDF. The stretchable materials as positive charged materials were also presented. This will make the TENG generate higher output power, compared with the PTFE-based TENG.