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The invention belongs to the technical field of composite material synthesis, and relates to a preparation method of Co3O4/PANI/MnO2 composite materials, in particular to a preparation method of a core-core-hull ternary composite material Co3O4/PANI/MnO2. According to the method, conventional materials Co3O4 and MnO2 which are low in cost, rich in resource and free of pollution are selected for use and synthesized with PANI with great conductibility, and then a core-core-hull heterostructure is designed successfully. Nickel foam serves as a current collector, a Co3O4 nanometer line array prepared according to a hydrothermal method serves as an inner core, a small part of capacitor is provided, Co3O4 serves as a framework, and a layer of PANI membrane is formed on the surface, where Co3O4 is generated, of the nickel foam through electrochemical deposition to serve as an outer core; a part of electric charges are stored for providing an effective approach for fast transmission of electronics, the conductivity of the material is improved, and finally, manganese dioxide prepared according to the hydrothermal method serves as a hull to further improve the capacitive performance of the material, so that the ternary composite material Co3O4/PANI/MnO2 which can be used for making a super capacitor electrode without binders is obtained.