A fine-quality, regular Cu-Mg-Al hydrotalcite-like compound was synthesized via the glycothermal method using CuCl2 \cdot 2H2O, MgCl2 \cdot 6H2O, AlCl3 \cdot 6H2O, and Na2CO3 as raw materials and sodium hydroxide as the precipitant. Hydrotalcite samples were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, thermogravimetric-differential thermal analysis, and Brunauer-Emmett-Teller N2 surface area measurements. The influence of glycol content on the characteristics of the sample was investigated. The results show that the glycol content in the system had a greater impact on regular hydrotalcite with an intercalated structure. A Cu-Mg-Al hydrotalcite-like compound with a well-defined shape, distinct intercalated structure, regular quality, and good dispersing capability could be obtained under the following conditions: glycol volume ratio of 10%, hydrothermal temperature of 180 °C, and reaction time of 15 h. The compound obtained was well crystallized and had the morphology of a homogeneous and hexagonal sheet. The thickness of each hexagon in the hydrotalcite was about 40 nm, which was consistent with the value estimated with the Scherer equation.