Magnesium aluminum layered double hydroxide (LDH) was synthesized by the co-precipitation method followed by calcination. The resulting materials were characterized by X-ray diffraction (PXRD) and attenuated total reflectance with Fourier transform infrared spectroscopy (FTIR/ATR) and simultaneous thermogravimetric analysis/differential scanning calorimetry coupled to mass spectrometry (TGA–DSC–MS). Calcined and non-calcined LDHs were used as adsorbents to remove azo dye Acid Green 68:1 in an aqueous solution. Adsorption experiment results indicated that calcined LDH possesses greater adsorption capacity (154.8mgg −1 ) than non-calcined LDH (99.1mgg −1 ). Isotherms showed that adsorption of the dye was more consistent with the Langmuir model. Kinetic experiments of calcined LDH adsorption showed that for low concentration (50, 100 and 200mgL −1 ), the system reached the adsorption equilibrium in 1, 2, and 4h, and for higher concentration after 10h. The best kinetic model was the pseudo-second order. Adsorption studies also showed that the capacity for adsorption of the dye by calcinated LDH does not significantly diminish with pH level variation.