The construction of electrode materials with rational morphology and structure based on bimetallic sulfides is crucial to improve the performance of supercapacitors. Ultra-thin three-dimensional nickel molybdenum sulfide nanosheet spheres (NiMo3S4 NSSs) are grown on nickel foam (NF) using a one-step hydrothermal synthesis. NiMo3S4 NSSs have a diameter of ~ 5 μm and nanosheet thickness of 200nm. The effects of increasing the hydrothermal synthesis time and molar concentration ratios of Ni2+ to MoO42- on the morphologies of the NiMo3S4 are investigated. Due to the synergistic effect of NiMo3S4 NSSs and bimetallic ions which can provide a larger solution contact areas and improve the redox activity, the electrode exhibits good electrochemical properties. The specific capacity of NiMo3S4 NSSs/NF electrode can reach 1002.4C/g (1A/g). After being assembled into a hybrid supercapacitor (HSC) with activated carbon (AC), the energy density can reach 72.1Wh/kg at the power density of 749.9W/kg. In addition, the HSC shows an excellent stability of 89% after 10, 000 charge-discharge cycles (10A/g).