Graphene oxide(GO)-chitosan composite hydrogels were successfully prepared via the self-assembly of chitosan molecules and GO. These as-prepared hydrogels were characterized by different techniques. The morphology of the internal network structure of the nanocomposite hydrogels was investigated. The adsorption capacity results demonstrate that the prepared GObased composite hydrogels can efficiently remove three tested dye molecules, Congo red, methylene blue and Rhodamine B, from wastewater in accordance with the pseudo-second-order model. The dye adsorption capacity of the obtained hydrogels is mainly attributed to the GO sheets, whereas the chitosan molecule was incorporated to facilitate the gelation process of the GO sheets. The present study indicates that the as-prepared composite hydrogels can serve as good adsorbents for wastewater treatment as well as the removal of harmful dyes.