A novel three-dimensional crumpled graphene oxide/cellulose nanocrystals (GO/CNCs) composite was successfully synthesized and firstly used as adsorbent for the removal of ionic liquid [BMIM][CI] from aqueous solution. The 3D crumpled structure and abundant oxygen of the functional groups on GO/CNCs composite can provide more chance for the sorption of [BMIM][CI] compared with CNCs and GO, respectively. Therefore, a series of batch experiments were carried out to evaluate the adsorptive property of 3D GO/CNCs composite towards [BMIM][CI], such as the GO mass content, the pH value and contact time. The results showed that pseudo-second-order kinetic model and Eovlich model were well fitted with the sorption kinetic. The isotherm adsorption data indicated that it was better described by Langmuir model, with the maximum sorption capacity of 0.455 mmol/g. This work provides a facile method for the preparation of 3D structure adsorbent from graphene oxide and cellulose nanocrystals which has high adsorption capacity of [BMIM][CI] in aqueous solution. (C) 2017 Elsevier B.V. All rights reserved.