We report for the first time the synthesis of Li4SiO4 by the modified combustion method, a rapid chemical process that takes 5 min for completion. This method uses nonoxidizer compounds instead of nitrate mixtures, which are not always commercially available. The effects of the following parameters on the production of Li4SiO4 were studied: (1) different lithium hydroxide:silicic acid:urea (LiOH:H2SiO3:CH4N2O) molar ratios; (2) the presence of air flow in the furnace chamber; and (3) the furnace heating temperature. It was found that LiOH:H2SiO3:CH4N2O molar ratios 6:13 heated at 1100 degrees C in the presence of additional air in the muffle chamber formed the best precursors to produce Li4SiO4.