Coupling ultrasmall Fe2O3 particles (~4.0 nm) with the MoS2 nanosheets is achieved by a facile method for high-performance anode material for Li-ion battery. MoS2 nanosheets in the composite can serve as scaffolds, efficiently buffering the large volume change of Fe2O3 during charge/discharge process, whereas the ultrasmall Fe2O3 nanoparticles mainly provide the specific capacity. Due to bigger surface area and larger pore volume as well as strong coupling between Fe2O3 particles and MoS2 nanosheets, the composite exhibits superior electrochemical properties to MoS2, Fe2O3 and the physical mixture Fe2O3+MoS2. Typically, after 140 cycles the reversible capacity of the composite does not decay, but increases from 829 mA h g-1 to 864 mA h g-1 at a high current density of 2 A g-1. Thus, the present facile strategy could open a way for development of cost-efficient anode material with high-performance for large-scale energy conversion and storage systems.