AbstractPbZrO3 (PZO)‐based antiferroelectric thin films are of great interest due to their high‐power density and fast charging and discharging capability. However, the problems of low breakdown strength and inferior energy storage density of PZO films have not been well solved. In this work, the insulating MgO as the blocking interlayer is inserted into PbZrO3 films (abbreviated as P/M/P), which can inhibit the electric charge transfer and enhance the breakdown strength, as well as regulation of the polarization behavior. The results show that the maximal endurable electric field is significantly improved, and the double‐hysteresis characteristic disappeared after introducing MgO blocking interlayer. The energy storage density of P/M/P films reaches 21.97 J/cm3 under 1700 kV/cm, accompanying an ultralow efficiency of 44.01% due to the severe polarization loss. Furthermore, low‐temperature annealing is performed to suppress the polarization loss, and an energy storage density of 17.27 J/cm3 accompanying a high efficiency of 75.53% is obtained at 3100 kV/cm, still exhibiting good stability after 1 × 107 fatigue cycles. This study demonstrates that combining the insulating interlayer and the low‐temperature annealing endow the PZO‐based films significantly improved energy storage properties, having great potential to be used in the dielectric capacitors.
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