The uncalcined glycerol-modified nanocrystallined Mg/AI layered double hydroxides (named as G-LDH) and calcined G-LDH (named as G-LDO) with molar ratio of Mg:Al = 3:1 were successfully synthesized using an easy and green hydrothermal method, and were characterized by scanning electron microscopy, transmission electron microscopy, N-2 Brunauer-Emmett-Teller surface area measurement, Fourier transformed infrared (FT-IR) spectroscopy and X-ray diffraction (XRD). The as-synthesized G-LDH and G-LDO were applied as adsorbents to remove methyl orange (MO) from aqueous solutions at different experimental conditions, and the results showed that the interaction of MO with G-LDH and G-LDO were strongly pH-dependent and ionic strength-independent. Kinetic study indicated the MO adsorption on G-LDH and G-LDO were well simulated by pseudo-second-order model. The MO adsorption on G-LDH and G-LDO were well simulated by Langmuir model, and the maximum adsorption capacity of G-LDO (q(max) = 1062.3 mg/g) was much higher than that of G-LDH (q(max) = 443.5 mg/g) at pH = 4.5. The thermodynamic parameters calculated from temperature-dependent isotherms indicated that the adsorption was spontaneous and exothermal process. The FT-IR and XRD analysis further evidenced that the interaction of MO with G-LDH was mainly dominated by electrostatic interaction, ion exchange, hydrogen bonding and surface complexation, whereas the uptake of MO to G-LDO was mainly attributed to electrostatic interaction and surface complexation. These results suggested that the G-LDO was a promising material for the efficient removal of organic pollutants in real environmental pollution cleanup. (C) 2016 Elsevier B.V. All rights reserved.