Herein, a facile and straightforward green-assembly approach was developed for preparation of nitrogen and sulphur co-doped three-dimensional (3D) graphene hydrogels (N/S-GHs) with the assistance of glutathione. Specifically, graphene oxide is reduced and assembled into 3D porous nanostructures with glutathione as the reducing agent and modifier for its intrinsic structure, along with the nitrogen and sulphur sources in the synthetic process. As expected, the as-obtained N/S-GHs demonstrated superior adsorption performances for organic dyes (e.g., methylene blue, malachite green, and crystal violet) in aqueous media. This work provides new insight for the green-assembly of 3D porous nanomaterials as adsorbent and their promising applications in water treatment. (C) 2016 Elsevier Inc. All rights reserved.