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Abstract Piezoelectric polymers hold great potential for various electromechanical applications, but only show low performance, with | d 33  | < 30 pC/N. We prepare a highly piezoelectric polymer ( d 33  = −62 pC/N) based on a biaxially oriented poly(vinylidene fluoride) (BOPVDF, crystallinity = 0.52). After unidirectional poling, macroscopically aligned samples with pure β crystals are achieved, which show a high spontaneous polarization ( P s ) of 140 mC/m 2 . Given the theoretical limit of P s,β  = 188 mC/m 2 for the neat β crystal, the high P s cannot be explained by the crystalline-amorphous two-phase model (i.e., P s,β  = 270 mC/m 2 ). Instead, we deduce that a significant amount (at least 0.25) of an oriented amorphous fraction (OAF) must be present between these two phases. Experimental data suggest that the mobile OAF resulted in the negative and high d 33 for the poled BOPVDF. The plausibility of this conclusion is supported by molecular dynamics simulations. 

In response to the stringent requirements for future DC-link capacitors in electric vehicles (EVs), it is desirable to develop dielectric polymer films with high-temperature tolerance (at least 105 °C) and low loss (dissipation factor, tan δ < 0.003). Although the biaxially oriented poly(ethylene terephthalate) (BOPET) film has an alleged temperature rating of 120 °C, its dielectric performance in terms of breakdown strength and lifetime cannot satisfy the stringent requirements for power electronics in EVs. In this work, we carried out a structure–electrical insulation property relationship study to understand the working mechanism for various PET films, including a commercial BOPET film, an amorphous PET (AmPET) film, and two annealed PET films (AnPET, i.e., cold-crystallized from AmPET). Structural analyses revealed a uniform edge-on crystalline orientation in BOPET with the a* axis in the film normal direction. Meanwhile, a high content of the rigid amorphous fraction (RAF) was identified for BOPET, which resulted from biaxial stretching during processing. On the contrary, AnPET films had a random crystal orientation with lower RAF contents. From dielectric breakdown and lifetime studies, the high-crystallinity AnPET film exhibited better electrical insulation than BOPET, and AmPET had the worst electrical insulation. Electrical conductivity results revealed that the high RAF content in BOPET led to reasonably high breakdown strength and long lifetime only at low temperatures (<100 °C). Meanwhile, PET crystals were more insulating than the amorphous phase, whether mobile, rigid, or glassy. In particular, the flat-on lamellae in the AnPET film were more effective than the edge-on lamellae in BOPET in blocking the conduction of charge carriers (electrons and impurity ions). This understanding will help us design high-temperature semicrystalline polymer films for DC-link capacitors in EVs.