The feasibility to synthesize, in large quantity, pure, and nontoxic tetrahedrite compounds using high-energy mechanical-alloying from only elemental precursors is reported in this study for the first time. Our processing technique allows a better control of the final product composition and leads to high thermoelectric performances (ZT of 0.75 at 700 K), comparable to that reported on sealed tube synthesis samples. Combined with spark plasma sintering, the production of highly pure and dense samples is achieved in a very short time, at least 8 times shorter than in conventional liquid-solid-vapor synthesis process. The process described in this study is a promising way to produce high-performance tetrahedrite materials for cost-effective and large-scale thermoelectric applications.