Aminoclay (AC), as a kind of layered silicates with positive charges, shows high dispersity in water and has been widely applied in the fabrication of intelligent hybrid hydrogel. Herein, heptakis-[6-deoxy-6-(2-sulfanylethanesulfonic acid)]-β-cyclodextrin (SCD), a kind of negatively charged cyclodextrin, was employed to construct the supramolecular hydrogel with aminoclay through the static electronic interactions, and the resultant SCD-AC hydrogel was fully characterized by means of X-ray powder diffraction (XRD), scanning electronic microscopy (SEM), fourier transform infrared spectroscopy (FT-IR), zeta potential, rheological test, etc. Significantly, the SCD-AC hydrogel can efficiently absorb not only I 3 ion in aqueous solution but also I 2 molecule in organic solvent, giving a high adsorption capacity up to 90% with 10 min.