Abstract: A heat dissipation structure and a synthesizing method thereof are provided by the present disclosure. The method comprises: providing a metal foil; forming a deposition substrate on a first surface of the metal foil, wherein the deposition substrate includes a barrier layer disposed on the metal foil and a catalyst layer disposed on the barrier layer, such that catalyst in the catalyst layer is prevented from diffusing into the metal foil; and synthesizing a carbon nanotube array on the deposition substrate formed on the first surface. The method provided by the present disclosure can increase density of the CNTs in the heat dissipation structure.