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Antiferroelectric thin-film capacitors with ultralow remanent polarization and fast discharge speed have attracted extensive attention for energy storage applications. A multilayer heterostructure is considered to be an efficient approach to enhance the breakdown strength and improve the functionality. Here, we report a high-performance multilayer heterostructure (PbZrO3/PbTiO3)n with a maximum recoverable energy storage density of 36.4 J/cm3 due to its high electric breakdown strength (2.9 MV/cm) through the heterostructure strategy. The positive effect of interfacial blockage and the negative effect of local strain defects competitively affect the breakdown strength, showing an inflection point at n = 3. The atomic-scale characterizations reveal the underlying microstructure mechanism of the interplay between the heterointerface dislocations and the decreased energy storage performance. This work offers the potential of well-designed multilayers with high energy storage performance t
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