Ni(Mg)Al-layered double hydroxides (LDH) were synthesized by coprecipitation. Structural properties of LDH and mixed oxides Ni(Mg)AlOx, obtained by LDH calcination, were studied by XRD and SEM. Textural properties of Ni(Mg)AlOx were studied by the nitrogen adsorption-desorption method. It was found that the formation of the single-phase LDH was occurred for any nickel content in the samples. The mixed oxides have a high specific surface area, the value of which decreases with increasing nickel content in the samples. Ni(Mg)AlOx are characterized by high activity in furfural hydrogenation. Selectivity of the formation of different reaction products depends on the nickel content in the catalysts. The full furfural conversion with the furfuryl alcohol selectivity no more than 65% was observed for the catalyst with a low nickel content. At the same time an increase in selectivity for furfuryl alcohol up to 84% occurs for the NiAl-catalyst with a furfural conversion not exceeding 43%. Display omitted •Synthesis of single-phase Ni(Mg)Al-layered hydroxides by coprecipitation.•Structural and textural properties of the Ni(Mg)Al-layered hydroxides and their calcined forms.•High activity of the Ni(Mg)AlOx catalysts in the reaction of aqua-phase furfural hydrogenation.•Selectivity of products formation can vary by changing the nickel amount in the Ni(Mg)AlOx catalysts.