The invention discloses a preparation method for a high-performance three-dimensional carbon nanotube composite negative electrode material. The preparation method comprises: by taking a carboxylated carbon nanotube as a three-dimensional network framework and taking a high-capacity material subjected to layer by layer self-assembly and modification as an active substance, uniformly mixing the carbon nanotube with the active substance under the action of electrostatic attraction; and then performing in-situ coating by taking a mixed element-containing N or S-doped carbon source as a three-dimensional coating layer, and performing high-temperature treatment to obtain the high-performance three-dimensional carbon nanotube composite negative electrode material. The invention furthermore discloses the high-performance three-dimensional carbon nanotube composite negative electrode material and an application thereof. According to the preparation method, the cycle performance of the active substance is remarkably improved, and the capacity of the composite material can be controllably adjusted by controlling a ratio of the carbon nanotube to the active substance. In addition, a solvent used in the method is water, so that the method is environmentally-friendly, good in repeatability and low in cost, and has relatively high potential of large-scale application and good industrialized prospects.