Substrate materials are of great significance for the development of pseudocapacitor electrodes. Herein, pseudocapacitive NiCo2O4 have been successfully grown on the 3D graphite felt (GF) substrate via a two-step method, including the prior co-deposition of Ni and Co ions on the GF and succeeding thermal transformation of Ni/Co precursors to spinel NiCo2O4. Porous NiCo2O4 nanosheets are formed on the surface of GF, yielding stand-alone nanocomposite electrodes. The experimental results show that the NiCo2O4/GF electrode achieves a remarkable specific capacitance of 2205 F g(-1) at a current density of 1 A g(-1), which remains 1790 F g(-1) when the current density is increased to 20 A g(-1). After cycling at a current density of 5 A g(-1) for 2000 cycles, the NiCo2O4/GF electrode still exhibits 90.7% of its original specific capacitance. Such encouraging rate capability and cycling stability of the NiCo2O4/GF electrode are attributed to the optimized structure of NiCo2O4 that functions synergistically with the underlying GF substrate to achieve excellent electron conductivity and enhanced ion diffusivity. Therefore, the as-synthesized binder-free NiCo2O4/GF electrode is a promising candidate for high-performance pseudocapacitors.