We demonstrate the construction of three-dimensional graphene oxide based gel networks through the self-assembly of a series of amphiphilic molecules, which possess a polar carbohydrate headgroup attached to a nonpolar pyrene group. The gelation process can occur in both aqueous and organic solutions and be influenced by the gelators' molecular structure. The driving forces for the gelation process were determined as π-π stacking and hydrogen bonding interaction by using fluorescence and infrared spectroscopies. Rheometry was used to investigate the mechanical properties of the hydrogels and the organogels. The hydrogel was investigated to be applied to remove dye from aqueous solution.