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The application of iron oxide as anode of lithium-ion batteries is hindered by its poor cycle stability, low rate performance and large voltage hysteresis. To address these problems, multi-channel surface modified amorphous Fe2O3 nanospheres were synthesized by using a facile hydrothermal method, which exhibited outstanding electrochemical performances. According to crystalline state and microstructure, it was found that surface structure of the amorphous Fe2O3 nanospheres can be controlled by adjusting the reaction time, due to the synergistic effect of ripening and hydrogen ion etching. Owing to the isotropic nature and the absence of grain boundaries, the amorphous Fe2O3 nanospheres could withstand high strains during the intercalation of lithium ions. Meanwhile, the multi-channel surface structure can not only increase the contact area between Fe2O3 nanospheres and electrolyte, but also reserve space for volume expansion after lithium storage, thereby effectively alleviating the volume change during the intercalation-deintercalation of lithium ions. As confirmed by the Galvanostatic intermittent titration analysis results, the amorphous Fe2O3 electrode had higher Li+ diffusion coefficient than the crystalline counterpart. As a result, the multi-channel surface modified amorphous Fe2O3 electrode exhibited higher specific capacity, more stable cycle performance and narrower voltage hysteresis. It is believed that amorphous metal oxides have great potential as high-performance anode of next-generation lithium-ion batteries.