The invention relates to the technical field of preparation of hydrotalcite-like compounds, and discloses a pure cobalt-like hydrotalcite compound and a preparation method thereof. Using the constant pH precipitation method, using cobalt nitrate as the cobalt source, methanol-water (volume ratio 1:1–8:1) mixed solution as the solvent, slowly add the cobalt nitrate solution to the sodium carbonate solution at room temperature and adjust the pH of the solution =8–12, after hydrothermal aging, suction filtration, washing, drying and other steps, pure cobalt-based hydrotalcites can be obtained. The hydrotalcite-like crystal phase is single, the structure is regular, and it presents a good layered structure and sheet morphology. The average thickness of the nanosheets is 5.9-12.8 nm, and it has a high degree of crystallinity. The preparation process of the invention is simple and easy to operate, the raw materials are cheap and easy to obtain, the preparation conditions are mild, the cycle is short, the purity and yield of the hydrotalcite-like stone are high, and the quantitative synthesis can be realized.