SiC single bulk crystals were grown using a high-temperature chemical vapor deposition (HTCVD) method, with SiH 4 and hydrocarbons as the source materials. SiH 4 is a pyrophoric gas, which frequently causes fatal accidents in experiments. In this study, therefore, we propose the use of a HTCVD method using tetramethylsilane (TMS), a cheap and safe precursor, for growing SiC bulk crystals. Although TMS contains C four times more than Si in its chemical formula, a stoichiometric SiC layer was successfully synthesized from TMS in the presence of a high concentration of H 2 based on the thermodynamic process design. 6H-SiC single crystals were successfully grown on a 6H-SiC seed crystal using the same process conditions. The resulting single crystalline layer was evaluated by rocking curve analysis by X-ray diffraction, which showed that the crystal properties of the grown SiC layer were improved compared to the seed crystals. This suggests that the TMS-based HTCVD method is feasible for practical use in SiC bulk growth.