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Exploring anode materials with an excellent electrochemical performance is of great significance for supercapacitor applications. In this work, a N-doped-carbon-nanofiber (NCNF)-supported Fe[sub.3]C/Fe[sub.2]O[sub.3] nanoparticle (NCFCO) composite was synthesized via the facile carbonizing and subsequent annealing of electrospinning nanofibers containing an Fe source. In the hybrid structure, the porous carbon nanofibers used as a substrate could provide fast electron and ion transport for the Faradic reactions of Fe[sub.3]C/Fe[sub.2]O[sub.3] during charge–discharge cycling. The as-obtained NCFCO yields a high specific capacitance of 590.1 F g[sup.−1] at 2 A g[sup.−1], superior to that of NCNF-supported Fe[sub.3]C nanoparticles (NCFC, 261.7 F g[sup.−1]), and NCNFs/Fe[sub.2]O[sub.3] (NCFO, 398.3 F g[sup.−1]). The asymmetric supercapacitor, which was assembled using the NCFCO anode and activated carbon cathode, delivered a large energy density of 14.2 Wh kg[sup.−1] at 800 W kg[sup.−1]. Additionally, it demonstrated an impressive capacitance retention of 96.7%, even after 10,000 cycles. The superior electrochemical performance can be ascribed to the synergistic contributions of NCNF and Fe[sub.3]C/Fe[sub.2]O[sub.3].