The chemical modification of self-assembled graphene hydrogels is a topic of emerging interest to harness the excellent physicochemical properties of two-dimensional (2D) graphene for macroscopic applications. We synthesized a series of mechanically strong and lightweight nitrogen (N)-doped graphene hydrogels (NGHs), with different doping concentrations, through a simple one-pot hydrothermal reaction and systematically evaluated their performance as both adsorbents and photocatalysts for environmental remediation. Acridine orange (AO) was chosen as a model pollutant. The successful incorporation of N atoms into the carbon lattice of the macroscale 3D graphene-based materials was verified by Raman spectroscopy, Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). Although the N content of the graphene macroassemblies varied inversely with doping density, a conspicuous increase in specific surface area was observed at all doping levels, resulting in a higher adsorption capacity and surface reactivity than the undoped hydrogel. The adsorption equilibrium was best represented by the Langmuir isotherm (with maximum monolayer coverage of 124 mg g(-1) at 25 degrees C) while the adsorption kinetics followed both the pseudo-first and pseudo-second order rate expressions. Further, the NGHs could effectively photodegrade 20 mg L-1 AO aqueous solution by almost 70% within 5 h of visible light irradiation. The fairly good photooxidative ability of the NGHs originates from the synergistic effect of N functionalization and 3D interconnected mesoporous network structure, leading to greater uptake of AO, better absorption of visible light and rapid spatial separation of photogenerated electron-hole pairs. (C) 2017 Elsevier B.V. All rights reserved.