One of the long-standing challenges of current lead-free energy storage ceramics for capacitors is how to improve their comprehensive energy storage properties effectively, that is, to achieve a synergistic improvement in the breakdown strength (E ) and the difference between maximum polarization (P ) and remnant polarization (P ), making them comparable to those of lead-based capacitor materials. Here, a polymorphic polar nanoregions (PNRs) structural design by first introducing 0.06 mol BaTiO into Bi Na TiO is proposed to construct the morphotropic phase boundary with coexisting structures of micrometer-size domains and polymorphic nanodomains, enhance the electric field-induced polarization response (increase P ). Then Sr(Al Ta )O (SAT)-doped 0.94 Bi Na TiO -0.06BaTiO (BNBT) energy storage ceramics with polymorphic PNRs structures are synthesized following the guidance of phase-field simulation and rational composition design (decrease P ). Finally, a large recoverable energy density (W ) of 8.33 J cm and a high energy efficiency (η) of 90.8% under 555 kV cm are obtained in the 0.85BNBT-0.15SAT ceramic prepared by repeated rolling process method (enhance E ), superior to most practical lead-free competitors increased consideration of the stability of temperature (a variation <±6.2%) and frequency (W > 5.0  cm , η > 90%) at 400 kV cm . This strategy provides a new conception for the design of other-based multifunctional energy storage dielectrics.

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