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In this study, a facile pyrolysis process is utilized to convert a mantis shrimp shell into a 3D bicontinuous porous, highly wrinkled, nitrogen-doped, graphene-like ultrathin carbon sheet (3D BWGC). The 3D BWGC achieves a high surface area of 2300 m2 g−1 and a pore volume of up to 1.63 cm3 g−1. The specific capacitance of the 3D BWGC in 0.5 M H2SO4 electrolyte is 370.9 F g−1 at a current density of 1 A g−1 and an operating voltage window of 1.1 V. By introducing Fe2+, the operating voltage window of 3D BWGC symmetric supercapacitors can reach 1.8 V in a neutral electrolyte, and a specific capacitance of 317.2 F g−1 can be obtained at a current density of 0.5 A g−1. Remarkably, the fabricated symmetric supercapacitors using 2 M MgSO4 + 0.05 M FeSO4 electrolyte demonstrated an energy density as high as 17.7 W h kg−1 at a power density of 180 W kg−1. The assembled supercapacitors exhibit good cycling performance, maintaining an initial capacitance of 87.2% over 30 000 cycles. These excellent performances indicate the promising prospects of 3D BWGC in high-performance electrochemical energy storage. [ABSTRACT FROM AUTHOR]