The invention discloses a preparation method of a polyhedral metal-organic framework compound ZIF-67. The preparation method comprises the following steps: preparing a solution from Co(NO3)2.6H2O, 2-methylimidazole and methanol, mixing and stirring, reacting at a normal temperature, performing centrifugal washing, drying and the like. The ZIF-67 presents bluish violet, is in the shape of rhombic dodecahedron, and has the particle size of 300-920nm. The prepared ZIF-67 is in the shape of rhombic dodecahedron, the particle size of the framework is small and uniform and can be controlled to be about 300nm, the specific surface area is large, and the overall distribution is uniform. The material disclosed by the invention is high in degree of crystallinity, has high specific surface area and porosity, homogeneous distribution can be formed, the prepared framework is small in particle size, and the overall distribution is uniform. Meanwhile, the compound is high in electric shock capacity and long in service life, has excellent lithium storage property, and can avoid attenuation after 200 charge-discharge cycles at most. The stability in the application is excellent, the condition thatthe current is unstable is avoided, and the product purity is high. The yield of the preparation method is high and can reach 70% or higher, and the preparation process is simple and feasible and worthy of market popularization.