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Polymer-based dielectrics have been attracted much attention to flexible energy storage devices due to their rapid charge-discharge rate, flexibility, lightness and compactness. Nevertheless, the energy storage performance of these dielectric polymers was limited by the weak dielectric breakdown properties. Crosslinked structure has been proven efficient to enhance breakdown strength ( E  b ) and charge-discharge efficiency ( η ) of polymer film capacitors. However, crosslinked networks usually lead to low electric displacement of dielectric capacitors, which greatly restrict their energy storage density ( U  d ). In this work, we present a tri-layered composite via layer-by-layer casting technology, where crosslinked polyvinylidene fluoride (c-PVDF) was used as the inter-layer to offer high breakdown strength, and the outer ternary fluoropolymer layers with high dielectric constant could provide high electric displacement. The optimal tri-layered composites exhibit an ultrahigh discharge energy density of 18.3 J cm -3 and a discharge efficiency of 60.6% at 550 kV mm -1 . This energy density is much higher than that of the PVDF terpolymer and commercially biaxially oriented polypropylene (BOPP, 1-2 J cm -3 ). The simulation results prove that the enhanced energy density originates from the effectively depressed charge transport in crosslinked structure at high applied electric field. Moreover, this work provides a feasible method for developing flexible all-organic high-energy-density composites for polymer capacitors.

Enhanced energy storage density of all-organic fluoropolymer composite dielectric via introducing crosslinked structure