Abstract Mg2Si1-xSnx thermoelectric compounds were synthesized through a solid-state reaction at 700 °C between chips of Mg2Sn-Mg eutectic alloy and silicon fine powders. The Al dopants were introduced by employing AZ31 magnesium alloy that contains aluminum. The as-synthesized Mg2Si1-xSnx powders were consolidated by spark plasma sintering at 650-700 °C. X-ray diffraction and scanning electron microscopy revealed that the Mg2Si1-xSnx bulk materials were comprised of Si-rich and Sn-rich phases. Due to the complex microstructures, the electrical conductivities of Mg2Si1-xSnx are lower than Mg2Si. As a result, the average power factor of Al0.05Mg2Si0.73Sn0.27 is about 1.5 × 10-3 W/mK2 from room temperature to 850 K, being less than 2.5 × 10-3 W/mK2 for Al0.05Mg2Si. However, the thermal conductivity of Mg2Si1-xSnx was reduced significantly as compared to Al0.05Mg2Si, which enabled the ZT of Al0.05Mg2Si0.73Sn0.27 to be superior to Al0.05Mg2Si. Lastly, the electric power generation from one leg of Al0.05Mg2Si and Al0.05Mg2Si0.73Sn0.27 were evaluated on a newly developed instrument, with the peak output power of 15-20 mW at 300 °C hot-side temperature.