MIL-68(Al), a powdered aluminum-based metal organic framework (MOF), was synthesized and used to explore its adsorption behavior toward methyl orange (MO). The adsorption isotherm, thermodynamics, kinetics, and some key operating factors as well as changes in the material's structure were investigated. The adsorption isotherm conformed to the Langmuir isotherm model and the maximum equilibrium adsorption capacity was 341.30 mg g−1. Thermodynamic data demonstrated that the adsorption process was spontaneous, endothermic and showed positive entropy. For kinetics, the process of MO adsorption onto MIL-68(Al) was more suitably described by a pseudo-second-order model. Electrostatic and hydrogen-bonding interactions contributed to dye adsorption, with electrostatic interactions considered to be the principal binding force between adsorbent and adsorbate. Furthermore, MIL-68(Al) maintained a stable structure after adsorption. From these results, MIL-68(Al) was suggested here to be a stable MOF adsorbent for removing MO from aqueous solution.