Three different well-defined Ni/Mg(Al)O catalysts for natural gas conversion are prepared and exposed to the dry reforming of propane reaction at 600 °C. The catalysts have in common that they are based on layered double hydroxides (LDH) as precursor material. Two of the catalysts, Cat-A and Cat-B, are prepared via a novel delamination–restacking route of single layer nanosheets whereas the reference catalyst, Cat-C, is obtained using earlier established bulk procedures. All three catalysts show stable performance at the selected catalytic testing conditions, and the intrinsic activity appears to be mainly correlated with the mean Ni particle diameter. The novel catalysts, based on the nanostructured LDH precursors, have similar performance as the high performing reference catalyst, indicating that the delamination–restacking process do not alter the catalytic properties of the final nanostructured material. The new preparation route is concluded to be suited for controlling design of well-defined metal-on-support model catalysts for single parameter studies.