We present the synthesis and structural characterization of new nickel-containing Mg-Al layered double hydroxides (LDH), which adopt a structure in which nickel, chelated with ethylenediaminetetraacetate to a divalent anion [Ni(EDTA)](2)-, is nested between brucite-like layers of LDH. The corresponding LDH-derived Ni-Mg-Al mixed oxides demonstrated high and stable catalytic function toward the reaction of methane reforming with carbon dioxide into synthesis gas at 800 degreesC. It is shown that the state of the supported nickel and the coke deposition process were significantly influenced by the method of catalyst preparation.