With the increasingly high requirements for wearable and flexible devices, traditional inorganic capacitors cannot meet the flexible demand of next-generation electronic devices. In this work, the energy storage property of all-inorganic flexible films has been systematically studied. PbZrO3 (PZO) and Al2O3 (AO) are selected as the antiferroelectric layer and insulating layer, respectively. The heterostructured films are prepared on the fluorphlogopite (F-Mica) substrate by chemical solution deposition. The microstructure, polarization behavior, and energy storage performances are investigated. The results demonstrate that the AO/PZO/AO/PZO/AO (APAPA) multilayered thin film possesses a greatly improved energy storage density (W rec) of 28.1 J/cm3 with an excellent energy storage efficiency (η) of 80.1%, which is ascribed to the enhanced breakdown strength and large difference in polarization. Furthermore, the capacitive films exhibit good stability under a wide working temperature range of 25–140 °C and an electric fatigue endurance of 107 cycles. Besides, the energy storage performances are almost unchanged after 104 bending cycles, demonstrating an excellent mechanical bending endurance. This work sheds light on the preparation technology and improvement of the dielectric energy storage performance for all-inorganic flexible multilayered thin films.

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