Sn2Fe/Al2O3/C nanocomposites are synthesized using a high-energy, mechanical milling method with thermally synthesized Sn2Fe, Al2O3 and carbon (Super P) powders. The effect of Al2O3 addition on the microstructure of the Sn2Fe/Al2O3/C nanocomposites is examined. The electrochemical characteristics of the material as an anode in lithium-ion batteries are also evaluated. High-resolution transmission electron microscopy shows that the crystallite size of active Sn2Fe in the Sn2Fe/Al2O3/C nanocomposite is smaller than that of the Sn2Fe/C nanocomposite without Al2O3. A decrease in the initial irreversible capacity and enhanced cycle performance of the Sn2Fe/Al2O3/C nanocomposite electrode are observed.