In the present study, we fabricated high purity and electrically machinable Ti3SiC2 ceramics by mechanical alloying and subsequent spark plasma sintering. The effect of a trace amount of Al on these synthesis processes was examined. Our results showed that Ti3SiC2 could be synthesized by high energy milling. Spark plasma sintering of mechanically alloyed powder at the temperatures of 1000-1200°C produced nearly single-phased Ti3SiC2 materials. The purity of the sintered Ti3SiC2 bulk was remarkably increased by addition of a small amount of Al. Ti3SiC2 with a purity of 99.3 wt% and a relative density of 98.9% was obtained by mechanical alloying and subsequent spark plasma sintering from a starting mixture composed of n(Ti) : n(Si) : n(Al) : n(c) = 3 : 1 : 0.2 : 2 at 1100°C.