Here, we report a method for facile gram-scale synthesis of tetrahedrite (Cu12Sb4S13) nanoparticles (NPs) with high quality and good reproducibility. The obtained NPs had a well-defined tetrahedral shape with a mean edge length of ∼70 nm. We sintered the NPs by the hot press technique to fabricate a nanostructured pellet for thermoelectric measurements. The figure of merit (ZT) value of the pellet was 0.52 at 675 K, which was comparable with the ZT value of the non-nanostructured counterpart.