Aluminum-containing ternary carbide, Al4SiC4, was successfully synthesized using a mixture of Al(OH)(3), SiO2, and phenolic resin by a carbothermal reduction process without any posttreatment. In addition, the processing parameters were optimized in this study. Unlike the JCPDS pattern of Al4SiC4, the powder has a highly aligned structure along the c-axis, indicating a hexagonal plate-like morphology. The growth rate of particulates was higher than the nucleation rate as the carbon content decreased. The crystallinity (formation yield) of Al4SiC4 was much more dependent on the ratio of carbon to oxides than on the ratio of SiO2 to Al(OH)(3). Possible reaction mechanisms responsible for the synthesis of ternary carbide are discussed by considering reactions at the initial and later stages during the carbothermal reduction process.