The invention relates to a method for forming a carbon composite structure by using carbon nano tube and graphene, which comprises the following steps: plating an aluminum film and an iron film in turn on a cleaned substrate; putting the treated substrate into a conventional chemical vapor deposition device, and depositing and growing a carbon nano tube array, wherein the height of the carbon nano tube array is 10 to 300 microns, the diameter of the carbon tube is 10 to 20 nanometers and the density is 1,010 to 1,011cm<2>; taking a graphite substrate, fixing the back of the graphite substrate on a plane, and splitting a flat upper surface; and reversely clasping the prepared multi-wall carbon nano tube array on the surface of the flat graphite, contacting the upper surface of the carbon nano tube array and the surface of the graphite, pressing the carbon nano tube array and the graphite, dragging a silicon substrate along the direction parallel to the surface of the graphite, and taking up the silicon substrate along the direction vertical to the surface of the graphite after the silicon substrate is dragged for 5 to 10 centimeters. Several to hundreds of graphene sheet layers are attached to the surface of the carbon nano tube so as to obtain the carbon composite structure. The method of the invention has the advantages of simple preparation, few required apparatus, high success rate, low cost and high speed.