Two-dimensional (2D) structures have received substantial attention in the energy applications. However, a common problem with 2D layered structures is restacking during the charge-discharge process. In this work, a graphene-like structure, molybdenum disulfide (S-MoS2), was synthesized using the hydrothermal method. Moreover, zero-dimensional (OD) alpha-Fe2O3 nanoparticles were constructed to act as a spacer in the slurry. Subsequently, the three-dimensional (3D) S-MoS2@Fe2O3 nanoparticles were fabricated by the ultrasonic vibration process to improve their electrochemical properties. On the basis of the 3D architecture, the alpha-Fe2O3 nanoparticles not only prevent the restacking of MoS2 sheets, but also increase accessibility for electrolyte penetration to provide more active sites and lower the diffusion energy barrier for Li(+)ions during the charge-discharge process. In the potential window of 3 V-0.01 V, high-rate charge-discharge and long cycle tests were performed to investigate the electrochemical performance of all electrodes. The electrochemical performance was enhanced through spatial distribution of MoS2. In summary, these S-MoS2@Fe2O3 nanoparticles possess high potential for application as anode materials in next-generation lithium-ion batteries.