It is expected that composites made of carbon nanotubes (CNT) and copper (Cu) display both mechanical and electrical properties, but the low damage dispersion and high-quality composite of high-content CNTs have always been research difficulties. In this paper, high-content CNTs/Cu composites were prepared. The effects of the sintering method, sintering temperature, directional rolling and the CNTs' content on the relative density, hardness and electrical conductivity of the composites were studied. The uniform dispersion of high-content CNTs in Cu matrix was achieved by ball milling, sintering and rolling, and the processes did not cause more damage to the CNTs. The properties of composites prepared by spark plasma sintering (SPS) and vacuum hot pressing sintering (HPS) were compared, and the optimum process parameters of SPS were determined. When the CNTs' content is 2 wt.%, the hardness is 134.9 HBW, which is still 2.3 times that of pure Cu, and the conductivity is the highest, reaching 78.4%IACS. This study provides an important reference for the high-quality preparation and performance evaluation of high-content CNTs/Cu composites.