This letter reports the thermoelectric properties of Bi-doped Mg2Si0.4Sn0.6 thermoelectric materials. It was found that the ZTs of this material could be greatly enhanced by Bi-doping. Analyses on the transport properties showed that the power factors of the material were enhanced while the lattice thermal conductivities were reduced by Bi-doping. The reduction of the lattice thermal conductivity was likely caused by the interstitial Bi impurities. A peak ZT ≈ 1.55 at 773 K was obtained.