We now report the preparation of alkylammonium-tetratitanate intercalation compounds with the aid of a macrocyclic compound, [2.2.2]-cryptand. The macrocyclic compound strongly interacts with the interlayer cation to promote the ion exchange reactions, which do not proceed in its absence. The formation of the intercalation compounds was confirmed by X-ray diffraction and elemental analysis. Since the present method is simple in operation, it is applicable to the preparation of a wide variety of inorganic-organic supramolecular systems.