The invention discloses a preparation method of a graphene-carbon nanotube compound film based on a three-dimensional network appearance. The method comprises the step of: transferring and stamping graphene and a carbon nanotube onto glass, a tantalum sheet, a silicon chip, a stainless steel plate or a polyethylene glycol terephthalate substrate in the mass ratio (1-10):1 through spraying deposition or vacuum suction filtration, wherein the grapheme is graphene oxide prepared by using an improved Hummers method; and a preparation method of a carbon nanotube solution comprises the following steps of: mixing acids; dispersing surfactants such as sodium lauryl sulfate, sodium dodecyl benzene sulfonate and hexadecyl trimethyl ammonium bromide in an auxiliary way, and the like. The graphene-carbon nanotube compound film prepared by adopting the method has the advantages of adjustable transmission and surface resistance, high uniformity, high stability, simple preparation method process and the like, and can be loaded on a rigid substrate as well as a flexible substrate.