In the present study, high-content Ti3AlC2 ceramic powders were fabricated by mechanical alloying (MA) using the Ti, Al and C as the starting materials. And the effect of Al content on the formation of Ti3AlC2 was investigated. The results showed that the large-sized granules were obtained to coexist with the powders after ball milling of 3Ti/Al/2C powder mixtures for 3 h. Ti3AlC2 in the synthesized powders is the main phase based on the XRD analysis. For the composition of 3Ti/1.1Al/2C, high-content Ti3AlC2 powders (87.6 wt.%) have been obtained after milling for 3h. Excessive Al, however, would reduce the content of Ti3AlC2 in the products.