A simple chemical method was employed to coat carbon nanotubes with a layer of copper. Due to the hydrophobic nature, large surface curvature, small diameter and large aspect ratio, it is difficult to gain continuous electroless plating layer on the surface of carbon nanotubes. In this paper, a series methods (oxidization, sensitization and activation) are used to add active sites before electroless plating, and the adjustment of the traditional composition of copper electroless plating bath and operating condition can decelerate electroless plating rate. The samples before and after coating were analyzed using transmission electron microscopy and energy-dispersive X-ray spectroscopy. The results showed that the surface of carbon nanotubes was successfully coated with continuous layer of copper, which lays a good foundation for applying carbon nanotubes in composites.