This work reports the preparation of two series of Ni-aluminosilicates by the sol-gel and the co-precipitation methods. The main difference between the two processes of synthesis is the pH of the initial mixture, 2 for the sol-gel and I I for the co-precipitation method, respectively. The obtained solids are heat-treated at various temperatures in the range of room temperature to 1000 degrees C, and the resulting materials are characterized by X-ray diffraction, thermogravimetric and differential thermal analysis, ultraviolet-visible spectroscopy, nitrogen adsorption, and transmission electron microscopy. Various nickel compounds crystallize under the sol-gel reaction conditions, as well as, amorphous silica and crystalline 2NaAlO(2)-3H(2)O. Ni-Al hydrotalcite, takovite, and amorphous silica are obtained when the samples from the co-precipitation method are analysed. A maximum of 302 m(2)/g Of Specific surface area shows the co-precipitation samples series, with only 32 m(2)/g in the case of the sol-gel samples series. The catalytic performance in the epoxidation of (Z)-cyclooctene at room temperature and atmospheric pressure is evaluated using aqueous hydrogen peroxide as oxidant. (c) 2006 Elsevier B.V. All rights reserved.