Dimensionality and rational design of electrode architectures play a crucial role in determining materials' fundamental properties and the electrochemical performance of supercapacitor. For a proof-of-concept, Ni–Co layered double hydroxides (LDH), NiCo2O4 and NiCo2S4 nanosheets supported on carbon fiber paper (CFP) substrate are prepared by simple hydrothermal methods in this work. When tested as the pseudo-capacitor positive electrode, the self-support nanosheets on CFP demonstrate good performance and rate capability as well as excellent cycling life, which contributes to the unique hierarchical nanosheets structure supported on 3D conductive CFP substrate with open permeable channels, facilitating electrolyte penetration and ensuring more efficient ion diffusion and faster electron transport. The asymmetric supercapacitor based on pseudocapacitance of both electrodes is further first realized by using NiCo2S4 nanosheets and FeOOH nanorods as positive and negative materials, respectively. The obtained device can deliver a maximum power density of 8.6kWkg−1 and energy density of 45.9Whkg−1 and even after 10000 reversible cycles at a cell voltage of 1.6V in aqueous electrolyte, there still retained 86.4% of its initial capacitance.