In this study, both uncalcined (MgNiAl-CO3) and calcined (MgNiAl-C) hythotalcites were used in the adsorption of methyl orange (MO) from aqueous solution as an anionic dye in a batch system. Various conditions such as initial dye concentration, adsorbent dosage, contact time, solution pH, and temperature were investigated. The adsorption kinetics was studied using classic equations of pseudo-first-order, -second-order and intraparticle diffusion models. The dynamical data fit well with the pseudo-second-order kinetic model. The positive value of the changes in enthalpy (Delta H degrees), the negative value of Gibbs free energy (Delta G degrees), showed that the adsorption is endothermic and spontaneous for all the studied temperatures. The equilibrium adsorption data were analyzed using three non linear adsorption models: Langmuir, Freundlich and Redlich-Peterson. The results showed that Langmuir and Redlich-Peterson isotherms fit the experimental results very well with high correlation coefficients. The Langmuir isotherm model exhibited a maximum adsorption capacity q(max) of 375 mg/g for the calcined MgNiAl-C. This result is of practical interest, with respect to the selection of sorbents, to optimize aquatic environment remediation technologies. (C) 2012 Elsevier B.V. All rights reserved.