Although graphene oxide (GO)-based materials are attractive media for water treatment, their separation from water for reuse remains a challenge. This study investigated the self-assembly of GO sheets in the presence of chitosan (CS), a natural polyaminosaccharide, into sponges. We found that about 93% of added CS could be combined with GO, regardless of the CS concentration. There exists an upper critical gelation limit, below which hydrogel forms and above which precipitation takes place. Results indicate that upon freeze-drying, a stable GO/CS sponge was generated only at a CS content of >= 9%. Sponges with CS content between 9% and 41% had good filtering performance. The sponges were characterized with XRD, SEM and FTIR measurements and the interaction between GO and CS was analyzed. The GO/CS sponge with CS content of 9% had adsorption capacity of 275.5 mg/g for methylene blue (MB), a model dye molecule. Both electrostatic attraction and hydrophobic interactions are responsible for MB adsorption by GO/CS sponges. The GO/CS sponge could be regenerated for repeated use using 0.5 M NaOH solution as desorption reagent. Our fixed-bed column studies illustrate that the GO/CS sponge performed well as a filtering material for removing MB from water. (C) 2018 Elsevier Inc. All rights reserved.