Lithium orthosilicate (Li4SiO4) powder was synthesized by the solid-state reaction of lithium oxide with amorphous silica, and the effects of fabrication parameters on the structural characteristics of the product were investigated. Processing considerations such as milling media, drying technique, calcination time and temperature, pressing behavior, sintering time and temperatures, and impurity concentration were addressed. The initial powder particle size was observed to be important in achieving high sintered density, with densities as high as 98% TD achieved with a particle size of approximately 1 μm.