Ti2AlC powders with high purity were successfully synthesized via high energy milling and heat treatment of Ti, C and Al powders. The effects of composition and thermal treatment on the formation and purity of Ti2AlC were examined in detail. The results shown a mechanically induced self-propagating reaction (MSR) was triggered to form Ti3AlC2, TiC and TiAlx during the high energy milling. When the as-milled powders were heat treated, Ti2AlC was initially formed by the reaction between TiAl and TiC. With continuously increasing temperature, Ti2AlC was also produced by the reaction between TiAl and Ti3AlC2.