We present a facile approach to make Al-Sb, carbon-modified (Al-Sb-C) nanocomposites for use as new anode materials in lithium-ion batteries (LIB). Alloying is achieved by one step synthesis using high energy mechanical milling (HEMM), producing nanometer-sized alloy particles, Sb-AlxCy-C. Based on electrochemical analyses, we determined that Sb acts as an active material, and both Al and carbon create a hybrid buffering matrix that mitigates the volume expansion of the active material during lithiation/delithiation to a greater degree as compared to that by a pure metallic matrix (AlSb). In addition, we optimized the stoichiometric ratio of Al and Sb concerning specific capacity and cycling performance. AlSb-C anodes also showed good rate capability and volumetric capacity. Overall, the new AlSb-C composite is a promising candidate for use as the negative electrode in lithium-ion batteries, providing an alternative to commercially available graphite electrodes.