In this work, both samples MgNiAl– LDH and MgNiFe–LDH hydrotalcites were utilized to remove the anionic dye Congo Red (CR) from an aqueous solution. Samples characterization was carried out by X-ray diffraction (XRD), infrared spectroscopy (IR) and Thermogravimetric/Differential Scanning Calorimetry (TG/ DSC). Various parameters were investigated, including the initial dye concentration, adsorbent mass, contact time, solution pH,
and temperature. Using classical pseudo-first-order, second-order, and intraparticle diffusion models, adsorption kinetics were investigated. The dynamical data fit well with the pseudosecond order kinetic model. The equilibrium adsorption data were analyzed using three linear adsorption models: Langmuir, Freundlich and Temkin. The findings showed that the Langmuir isotherm adequately predicts experimental results with an ideal correlation coefficient. The isothermal Langmuir model revealed a maximum adsorption capacity of qmax of 5548 mg/g for the MgNiFe–LDH and of 4043mg/g for MgNiAl-LDH. This result is very useful when selecting sorbents to improve removal technology in the aquatic environment