The mechanically induced self-propagating reaction (MSR) and hot-pressing consolidation were adapted to synthesize Ti2AlC and Ti3AlC2 using Ti, C and Al powder mixtures. The effects of Al content on the microstructure and mechanical properties of fully dense Ti2AlC and Ti3AlC2 were investigated. The results reveal that the Ti3AlC2, TiC and TiAlx transitional phases were formed by mechanically alloying according to the mechanically induced self-propagating reactions (MSR). Through hot pressing the as-milled powders with initial composition of 2Ti/1.5Al/C and 2Ti/Al/C, respectively, at 1100°C for 1 h, the desired high purity Ti2AlC and Ti3AlC2 were produced. SEM images confirmed that the as-fabricated Ti2AlC and Ti3AlC2 grains are plate-like with nanoscale layered structure and dispersed uniformly.