For both C7H8 and CH4 processes, a transition of growth orientation can be observed. At the Raman spectra of deposited 3C-SiC coatings shows a Raman shift deviation of ± 1 cm -1 in both 1 st order 3C-SiC transverse optical (TO) and longitudinal optical (LO) mode. The Raman shifts for 1 st order TO and MO modes of bulk 3C-SiC are reported to be 796 cm -1 and 972 cm - 1 , respectively . On the other hand, an even higher deviation of Raman shift for 1 st order TO and MO modes is observed in the 3C-SiC coatings prepared with C7H8 with the corresponding TO at 794± 2 cm -1 and LO at 967± 2 cm -1 . The 2 nd order TO and LO modes of 3C-SiC 26 at 1520 cm -1 and 1710 cm -1 , respectively, are also detected in both processes. Moreover, at lower temperatures (C7H8: T < 1200 o C, CH4: T ≤ 1200 o C), broadened transverse acoustic (TA) and longitudinal acoustic (LA) modes of 3C-SiC, which are normally located between 150 and 600 cm -1 , are observed, indicating the existence of smaller SiC crystallites . However, at T ≥ 1300 ℃, the characteristic Raman modes for carbon phases, e.g. D-band at 1350 cm -1 , G-band at 1580 cm -1 and 2D band at 2701 cm - , are observed in the 3C-SiC samples prepared with C7H8, indicating the co-deposition of pyrolytic carbon. It is noteworthy that the appearance of these Raman peaks is observed at the same temperature as the shift from <111> to <110> oriented growth. This could be caused by the breakdown of the toluene molecules forming highly reactive intermediates at such high temperatures. It could also be possible that the Si precursor is depleted faster than the C precursor, leaving excess carbon species in the coating.