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Abstract Polyaniline‐capped mesoporous carbon nanosheets with high conductivity and porosity are synthesized by vapor deposition polymerization. The mesoporous carbon template is prepared by removing ordered cubic iron oxide nanocrystals embedded in the carbon matrix obtained by thermal decomposition of an iron‐oleate complex in a sodium chloride matrix. The evaporated aniline monomers are slowly polymerized on the carbon surface pretreated with FeCl3 as an initiator, partially filling the carbon pores to improve conductivity. The resulting products exhibit efficient hybrid energy storage mechanisms of electric double‐layer capacitance and pseudocapacitance. When the nanosheets are assembled for a symmetric supercapacitor, the device capacitance reaches 107.8 F g−1, at a current density of 0.5 A g−1, and a capacitance retention of 69.6% is achieved at a ten times higher current density of 5 A g−1. Electrochemical impedance spectroscopy reveals that the transition from resistive to capacitive behavior occurs within 0.63 s, indicating that fast ion and charge transport results in high capacitance and rate capability. The corresponding energy and power densities are 9.59 Wh kg−1 and 200.1 W kg−1 at a current density of 0.5 A g−1, demonstrating efficient energy storage in a symmetric supercapacitor.