In this paper, we describe a general process for the synthesis of highly crystalline Zn-Ni-Al hydrotalcitelike materials. The structure and thermal decomposition of the prepared samples are studied by XRD, FT-IR, TG-DSC, SEM, TEM and N 2 adsorption/desorption. The morphology of large-sized, porous and hexagonal platelike Zn-Ni-Al hydrotalcite is affected by calcination temperature. BET specific surface area and pore volume are observed to increase with increase of the calcination temperature up to 700 • C followed by a further decrease with increasing temperature.