Mesoporous nickel intercalated aluminosilicate nanohybrid has been synthesized through a recombination reaction between the colloidal suspension of exfoliated montmorillonite nanosheets and aqueous nickel acetate solution. According to powder X-ray diffraction and field emission-scanning electron microscopic analyses, the intercalation of nickel species expands significantly the basal spacing of the host montmorillonite clay and the crystallites of the intercalation compound are assembled to form a house-of-card structure. N-2 adsorption-desorption isotherm measurements with BJH pore analyses clearly demonstrated that the porosity of the intercalate originates mainly from mesopores (diameter similar to 50 angstrom) formed by the house-of-card type stacking of clay crystallites. From FT-IR and X-ray absorption spectroscopic analyses, it becomes certain that intercalated nickel ion is stabilized in an isolated NiO6 Octahedral unit. The present mesoporous intercalation compound is expected to be applicable as efficient catalysts or absorbents.