The invention relates to the technical field of preparation of hydrotalcite-like compounds, and discloses a pure cobalt hydrotalcite-like compound and a preparation method thereof. A constant pH precipitation method is adopted, cobalt nitrate serves as a cobalt source, a mixed solution of methyl alcohol and water (the volume ratio is 1: 1-8: 1) serves as a solvent, the cobalt nitrate solution is slowly dropwise added into a sodium carbonate solution at the room temperature, the pH of the solution is adjusted to be 8-12, and the pure cobalt hydrotalcite is obtained through the steps of hydrothermal aging, suction filtration, washing, drying and the like. The hydrotalcite-like compound is single in crystalline phase, regular in structure and good in layered structure and flaky morphology, the average thickness of nanosheets ranges from 5.9 nm to 12.8 nm, and the high crystallinity degree is achieved. The preparation process is simple and easy to operate, the raw materials are cheap and easy to obtain, the preparation conditions are mild, the period is short, the purity and the yield of the hydrotalcite-like compound are high, and quantitative synthesis can be realized.