Herein, Mg-Al layered double hydroxide (LDH) was firstly prepared by a water-in-oil microemulsion method and the prepared LDH sample was further calcined at different temperatures. The calcined LDH samples were carefully characterized using XRD, nitrogen adsorption, TEM, TGA, XPS, FTIR and zeta potential measurement. Calcined and uncalcined LDHs samples were used as adsorbents to remove orange II (O-II) dye in water. Adsorption experiments indicated calcination temperatures had an obvious 10 influence on the adsorption affinity of LDH, and the 500 º C calcined LDH sample (LDH-500) exhibiting the maximum adsorption capacity of 602 mg/g larger than that of LDH (224 mg/g). The pseudo-secondorder model was the best kinetic model to describe O-II adsorbed on the surface of the adsorbent, and the dye adsorption was well fitted using the Langmuir model for the prepared samples. The adsorption mechanism of O-II dye onto the calcined and uncalcined LDHs samples was mainly related to 15 electrostatic interaction between the anionic O-II molecules and positively charged surface of the adsorbents, and the slow intercalation of O-II into the layers of LDH and reconstruction of LDH-500.