Layered double hydroxides (LDHs) with Mg/Co/Aland Ni/Co/Al were synthesized for the first time by the urea hydrolysis method. The experimental conditions promoted aluminum rich and crystalline materials. The formation of LDHs was investigated by powder X-ray diffraction (XRD), chemical analysis, solid state nuclear magnetic resonance with magic angle spinning (Al-27-MAS-NMR), simultaneous thermogravimetric/differential thermal analysis (TGA/DTA), FTIR spectroscopy, scanning electron microscopy (SEM), and N-2 adsorption desorption experiments. A single phase corresponding to LDH could be obtained in all the investigated compositions. Thermal calcination of these LDHs at 500 degrees C resulted in the formation of solid solutions in which Al3+ was dissolved. All the calcined materials have rock-salt like structures and high surface areas. (C) 2014 Elsevier Ltd. All rights reserved.