We have attempted to synthesize the meixnerite (Mg–Al–OH) type layered double hydroxide (LDH) by a two step milling operation of a mixture of Mg(OH)₂ and Al(OH)₃ with water. In the first-step, a mixture of the starting materials was milled for 1 h without water, and the product prepared in the first-step was milled for 2 h with water in the second-step milling operation. The milled products were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR), and thermo gravimetric-differential thermal analyses with mass spectroscopy (TG-DTA/MS). The surface morphology was characterized by scanning electron microscopy (SEM). Meixnerite with a small amount of carbonate was successfully synthesized mechanochemically at ambient conditions by milling for only 3 h in a planetary ball mill.