The InSe β-CD FeSO 4 clathrate with hierarchical architecture reveals a giant magnetoresistive effect and extraordinary (oscillating) behavior of the current-voltage characteristics in the magnetic field in the direction perpendicular to nanolayers. A new technological approach for the synthesis of multilayered nanostructure is proposed. It allows attaining a fourfold degree of expansion of the initial InSe semiconductor matrix in which the cavitate of β-cyclodextrin (β-CD) and iron sulfate served as a guest content. This makes it possible to develop a theoretical model to describe the interlayer magnetoconductivity in such extremely anisotropic 2D layered compounds. Graphic dependencies of oscillating magnetoconductivity are analysed for different values of quantizing magnetic field in a layered structure whose interlayer transfer integral can be controlled artificially.