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A series of ferroelectric polarization reversal measurements have been conducted on spin-coated ultrathin poly(vinylidene fluoride-trifluoroethylene) [P(VDF-TrFE)] copolymer films sandwiched with different electroactive materials between P(VDF-TrFE) and metal electrodes. Three types of electroactive interlayers, including highly polarizable material copper-phthalocyanine (CuPc), electron conductive polyethylene dioxythiophene/poly(styrene sulfonate acid), and ion (proton) conductive poly (vinyl phosphonic) acid, have been employed in our experiment. In addition, the ferroelectric film with CuPc exhibits larger remnant polarization and the enhancement of fatigue resistance although higher drive voltage and more switching time can be observed, which differs from the samples with electron and proton conductors as interlayers. The further analysis shows that this may be attributed to higher dielectric constant of CuPc than that of P(VDF-TrFE) layer. These results suggest that three types of interlayers can lead to a large improvement of ferroelectric switching, which is promising for potential applications.