In this study, we presented the efficiently adsorptive removal of organic dye, methyl orange (MO), from aqueous solution with the hydrothermal synthesized Mg-Al layered double hydroxide (LDH). The as-obtained product was characterized by X-ray diffraction (XRD), Fourier transformation infrared spectroscopy (FTIR), and scanning electron microscopy (SEM). The adsorption characteristics of MO onto the Mg-Al LDH were evaluated in a batch adsorption process and systematically investigated by different experimental parameters, such as initial dye concentration, contact time, and solution pH. The adsorption kinetics were analyzed by pseudofirst-order, pseudosecond-order, Elovich, intraparticle diffusion, and Boyd models, which were well-described by the pseudosecond-order model. The equilibrium adsorption data were interpreted using the Langmuir, Freundlich, and Temkin isotherm models, which fitted well to both the Langmuir and Freundlich models. The monolayer adsorption capacity of the Mg-Al LDH toward MO was found to be 0.453 mol.kg(-1). These findings suggested that the LDH could be regarded as a promising adsorbent for the removal of anionic dye in wastewaters.