The present invention relates to a complex comprising a covalent organic framework (COF) synthesized on the surface of a carbon structure, a preparation method therefor, and use thereof, and specifically to a complex of a carbon structure and a covalent organic framework, wherein the specific surface area or pore volume of the covalent organic framework synthesized on the surface of the carbon surface is larger than the specific surface area or the pore volume of the covalent organic framework prepared without the carbon structure; a preparation method therefor; and use thereof.