In this paper, NiMoO4 electrode materials doped with different concentrations of Nd rare earth metals were prepared by sol–gel method. Its morphology, structure, and spectral analysis were characterized by different scanning instruments, and the experimental results show that the NiMoO4 electrode material after adding 0.5% Nd doping showed excellent capacitance performance, with a specific capacity of 2182 F/g at a current density of 1 A/g. The capacitance retention was still 98.5% after 10,000 cycles at a current density of 5 A/g, which has a better electrochemical performance compared with the NiMoO4 material with superior electrochemical performance. In addition, an asymmetric capacitor device was prepared using 0.5% Nd-NiMoO4 material and CNTs as positive and negative electrodes, respectively, and the device showed a high energy density of 73.5 Wh/kg. In addition, the capacitor device still had a capacitance retention of 91.9% after 10,000 cycles. This paper provides an effective reference route for the preparation of rare-earth-doped bimetallic oxide electrode materials.