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Lead-free dielectric relaxor ferroelectric (RFE) ceramics are one of the promising materials for dielectric energy storage applications. However, the contradiction between high polarization and low hysteresis leads to interior energy storage performance, which greatly limits their applications in high/pulsed power systems. Here, we propose an effective strategy to significantly improve the energy storage properties of 0.94Bi0.5Na0.5TiO3–0.06BaTiO3 (0.94BNT–0.06BT) with a morphotropic phase boundary (MPB) composition by constructing multiscale polymorphic domains and local heterogeneous structures. The introduction of Nd(Mg1/2Hf1/2)O3 (NMH) facilitates the formation of short-range ordered polar nanoregions (PNRs). Moreover, small amounts of nanodomains with high polarization are resulted from local heterogeneous structures with Bi- and Ti-rich regions. Multiscale polymorphic domains with the coexistence of rhombohedral/tetragonal (R+T) nanodomains and PNRs ensure both high polarization and low hysteresis, which is crucial for improving the energy storage performance. Furthermore, the excellent electrical insulation is resulted from the high insulation resistivity, grain size at the submicron scale and a wide band gap by NMH doping. Therefore, a high recoverable energy density (Wrec) of 7.82 J/cm3 with an ultrahigh efficiency (η) of 93.1% is realized in the designed BNT–BT–NMH ternary system because of both a large ΔP and high Eb. These findings, together with good temperature/frequency/cycling stability, indicate that the optimum composition ceramics are very promising materials for energy storage applications in high/pulsed power systems.
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