Abstract: A method for connecting graphene and metal compound electrodes in a carbon nanotube device through carbon-carbon covalent bonds, the method including: 1) providing a substrate, designing and preparing pre-patterned metal membrane electrodes on the substrate; 2) mixing carbon nanotubes with a volatile organic solvent to yield a dispersed suspension solution, disposing the carbon nanotube between the pre-patterned metal membrane electrodes in the dispersed suspension to allow two ends of the carbon nanotube to connect to the metal membrane electrodes, to form a carbon nanotube device; 3) annealing the carbon nanotube device under a mixture of nitrogen and argon, etching, by metal atoms, a part of carbon atoms at two ends of the carbon nanotube connected to the metal membrane electrodes to form notches; and 4) using hydrocarbon gas as a carbon source, and performing a chemical vapor deposition process.