Supermolecular hydrogels were prepared by alpha-cyclodeatrin (alpha-CD) and Tyloxapol, which can be considered as an oligomer of the nonionic surfactant polyoxyethylene tert-octylphenyl ether (TX-100) with a polymerization degree below 7. Two carbon materials, graphene oxide (GO) and graphene, were mixed into the alpha-CD/Tyloxapol hydrogel to adjust the physicochemical properties of hydrogel. In order to get stable graphene dispersion and then mix it with alpha-CD/Tyloxapol hydrogel, both TX-100 and Tyloxapol were used to disperse graphene for comparison. Interestingly, it can be found that TX-100 could disperse graphene better than Tyloxapol owing to smaller molecular size of TX-100 compared with Tyloxapol. Then, both the alpha-CD/Tyloxapol/GO and alpha-CD/Tyloxapol/graphene hydrogels were characterized by transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), Fourier transform infrared (FT-IR) spectroscopy, small angle X-ray scattering (SAXS), X-ray diffraction (XRD) and Theological measurements. The results revealed that the addition of carbon materials into alpha-CD/Tyloxapol hydrogel can change their microstructures and the Theological properties. Furthermore, it can be confirmed that a little amount of carbon materials could induce fluorescence quenching sharply which could be a promising candidate for optical sensor. (C) 2016 Elsevier Inc. All rights reserved.