Magnesiothermic reduction of silicon oxide can result in the formation of nanostructured, mesoporous elemental silicon (mp-Si), which has been explored in a variety of energy applications such as Li-ion battery anodes, photocatalytic water splitting, CO 2 reduction, drug delivery vehicles, and sensors as well as for gas storage. The physical properties of the resultant mp-Si generated via magnesiothermic reduction, and thus the potential utility, are highly dependent on the specific reduction conditions utilized. Herein, we report a modified magnesiothermic reduction method which allows for the synthesis of high surface area mp-Si nanoparticles. The reaction was initiated at 650 °C and then cooled to a lower temperature to minimize heat-induced morphological damage. The nanoparticles were characterized by using powder X-ray diffraction, scanning and transmission electron microscopies, and N 2 adsorption isotherm measurements. Particles prepared by using two-step annealing with the initial processing condition of 650 °C for 30 min followed by 300 °C for 4 h resulted in crystalline and completely reduced mp-Si with a high specific surface area of 542 ± 18 m 2 /g. mp-Si nanoparticles generated by using these specific parameters were further used for stoichiometric CO 2 conversion to CH 3 OH, and the reaction yields were 2.5 times higher than prior reports, demonstrating usefulness in effecting an important chemical transformation.