In this work, we test this hypothesis and demonstrated the possibility of controlling the preferred growth orientation of polycrystalline 3C-SiC between <111> and <110> by using either toluene or methane as carbon precursors in SiCl4-based SiC CVD. Furthermore, by quantum chemical calculations we show how the adsorption behavior of benzene and methyl group differs when they approach the 3C-SiC (111) and (110) surfaces.