(Zhang Q)) ty, and strong mechanical strength [13−16]. For example, Banerjee et al. [17,18] successfully achieved the preparation of various hydrogels that can be used as dye-adsorbing agents in waste-water removal. In addition, this group has also reported metal-nanoparticle-containing GObased hydrogels and novel morphological transformation of graphene based nanohybrids [19−21]. Generally, GObased composite hydrogels were obtained by mixing organic macromolecules or small amphiphiles with an aqueous GO dispersion [22−24]. Chitosan (CS), a well-known compound of chitin N-deacetylation, shows many eco-friendly properties, such as biodegradation, good biocompatibility, and antifungal activity. These characteristics make it a promising candidate in the fields of catalysis, materials, food, drugs, etc. [25−27]. Since GO crosslinks with chitosan via the carboxyl, hydroxyl, epoxy, and amine groups of chitosan, the adsorption capacity of the formed composite is expected to be high. To date, some reports have been published on GO-chitosan nanocomposites used for drug release and antimicrobial activity [28−32].In this study, we report the preparation of GO-based composite hydrogels using the self-assembly of CS and GO, and an in situ reduction approach. The composite hydrogels consist of both hydrogen bonding and electrostatic interactions between the CS molecules and GO sheets. CS molecules were incorporated to facilitate the gelation process of GO sheets, and the dye adsorption capacity of the hydrogel was mainly attributed to the GO sheets. For the three dyes tested in this study, namely, Congo red (CR), methylene blue (MB), and Rhodamine B (RhB), the as-prepared composite hydrogels exhibit good removal rates in accordance with the pseudo-second-order model. More importantly, the hydrogels prepared in this study have potential large-scale applications in organic dye removal and 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.