a b s t r a c tCu-Al layered double hydroxides (LDHs) with [Cu]/[Al] ratio 2 adopt a structure with monoclinic symmetry while that with the ratio 0.25 adopt a structure with orthorhombic symmetry. The poor thermodynamic stability of the Cu-Al LDHs is due in part to the low enthalpies of formation of Cu(OH) 2 and CuCO 3 and in part to the higher solubility of the LDH. Consequently, the Cu-Al LDH can be decomposed thermally (150 1C), hydrothermally (150 1C) and reductively (ascorbic acid, ambient temperature) to yield a variety of oxide products. Thermal decomposition at low (400 1C) temperature yields an X-ray amorphous residue, which reconstructs back to the LDH on soaking in water or standing in the ambient. Solution decomposition under hydrothermal conditions yields tenorite at 150 1C itself. Reductive decomposition yields a composite of Cu 2 O and Al(OH) 3 , which on alkali-leaching of the latter, leads to the formation of fine particles of Cu 2 O (o1 mm).