Abstract: A series of ferroelectric polarization reversal measurements were conducted on spin-coating ultrathin poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE)) copolymer films sandwiched with different electroactive materials between P(VDF-TrFE) and metal electrode. Three types of electroactive interlayers, including highly polarized material copper-phthalocyanine (CuPc), electron conductor poly(ethylene dioxythiophene)-poly(styrene sulfonate acid)(PEDOT-PSSH) and ion proton conductor poly(vinyl phosphonic) acid (PVPA) were employed. Results showed that the compensated charges from electroative interlayers, such as electrons, protons, as well as dipoles, would improve the fatigue behaviors of electronic devices.