A series of Cu-Al hydrotalcite-like layered compounds has been synthesized by coprecipitation using metal nitrate precursors and sodium carbonate. The Cu/Al atomic ratio was varied between 0.5 and 4. The dried precipitates were characterized by powder X-ray diffraction (XRD) and thermogravimetric analysis (TGA). The crystalline hydrotalcite-like phase was present as major component in all precipitates, the first time such crystalline phase was observed in the precipitates of the constituent metals ratio as low as 0.5. The malachite phase was also observed in variable amounts, and it became amorphous at low copper content.