A method for printing a CNT three-dimensional structure is disclosed. The present invention provides a method for preparing a CNT composite structure, comprising the steps of: providing, to a nozzle, an ink in which a CNT composite comprising CNTs and a flow control agent; positioning the nozzle at a predetermined point on a substrate; and printing a CNT composite pattern corresponding to the movement path of the nozzle by moving the nozzle along a predetermined path on the substrate while discharging the ink from the nozzle, wherein in the step of printing a CNT composite pattern, the pattern is stacked as the CNT composite by the evaporation of a solvent within the meniscus formed by the ink to be discharged from the nozzle between the nozzle and the substrate. According to the present invention, a CNT structure comprising CNTs as a main component can be prepared, a pattern can be continuously formed by a pressureless method without the clogging of a nozzle or the cutting off of ink, and the prepared CNT st
