Synthesis of trimethylchlorosilane by a catalytic redistribution reaction between methyltrichlorosilane and low-boiling products from the direct synthesis of methylchlorosilanes on 1-butyl-3-methylimidazolium chloroaluminate ionic liquids was investigated. The effects of experimental parameters, such as composition and loading of the ionic liquid catalysts, composition of reactants, and reaction temperature and time, on the redistribution reaction were studied in detail. Among the ionic liquid catalysts, [BMIM]Cl-3AlCl(3) showed high catalytic activity in the redistribution reaction toward the formation of trimethylchlorosilane with a maximum yield of 72.5% at a lower reaction temperature of 60 C. The conversions of the main reactants, such as methyltrichlorosilane and tetramethylsilane, were ca. 100%. The ionic liquid catalyst was easily separated from the reaction mixtures by the facile decantation method and exhibited good recycling performance in the redistribution reaction. In addition, the possible reaction route was also discussed.