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The growth mechanism of metal-free carbon nanotube (CNT) arrays on SiC surface was investigated systematically using high temperature annealing of 6H-SiC(000-1) crystals under various atmospheres, including inert, hydrogen-containing, and oxygen-containing environments.Carbon nanowall structure forms under the inert and hydrogen-containing atmospheres, while vertically aligned CNT arrays can be obtained in oxygen-containing atmospheres, such as H2O.The comparative studies reveal that oxygen-containing species play a critical role in the formation of CNTs on SiC.The transient SiO clusters formed at the C/SiC interface are proposed to be the active sites for CNT growth on SiC.