The preparation of three-dimensional honeycomb nitrogen-doped carbon materials (3D-HNCMs) which can be used as electrode materials for supercapacitors is reported. The composites with the 3D honeycomb structure exhibited better electrochemical performance, and the structure and properties were proved by various means, such as SEM, TEM, IR, N2 sorption, XRD and XPS. Used as electrode materials for supercapacitors in the KOH electrolyte, 3D-HNCMs displayed a significantly high specific capacitance (409 F/g at a current of 0.5 A/g). Moreover, the 3D-HNCM electrode exhibited superior electrochemical performance, such as excellent cycling stability (98% capacitance retention after 10,000 cycles), a maximum energy density of 15.37 W h/kg, a maximum power density of 40.3 kW/kg, and low equivalent series resistance (2.1 Ω). Particularly, the electrochemical characteristic of 3D-HNCMs could be attributed to the synergistic effect of a high surface area, unique microporous and mesoporous structure, and nitrogen atom doping. These carbon materials with unique structure are promising electrode materials for future supercapacitor application.