The adsorption of textile dyes onto Layered Double Hydroxides (LDH) and their thermally decomposed products is a promising strategy for the treatment of contaminated effluents-combining high removal efficiency with reasonable cost. The main purpose of this paper was to investigate the adsorption of textile azo dye Acid Yellow 42 (AY) onto calcined and uncalcined Mg-Al-CO 3-LDH. A set of analytical techniques was used to characterize the materials, namely X-ray diffraction (XRD), Attenuated Total Reflectance Fourier Transform Infrared Spectroscopy (ATR-FTIR), thermogravimetric analyses (TGA), N 2 adsorption-desorption isotherms and Scanning Electron Microscopy (SEM). In the study of azo dye adsorption, the following factors were assessed: kinetics, adsorption capacity, effect of temperature, initial pH value, and recyclability of the adsorbent material. The adsorption capacity of calcined LDH (CLDH) was almost four times greater than that of the LDH precursor: 1266 mg•g −1 (1.669 mmol•g −1) and 330.0 mg•g −1 (0.4350 mmol•g −1), respectively, at pH equal to 7.0 and 25°C. The greater adsorption capacity for CLDH is related to the recovery property of these materials in light of the so called "memory effect", which allows an intercalation process of the anionic dye, as demonstrated by XRD data.