The formation of inorganic adsorbent, nickel/aluminium-layered double oxide prepared by calcining nickel/aluminium-layered double hydroxide at 400 °C for 120 min using as dye adsorbent, was verified by XRD pattern, SEM image, as well as FTIR and UV-visible spectra. The calcined product showed higher removal efficiency than that of the uncalcined one resulting from larger surface area and pore volume, and memory effect. The different charge of dye molecules was an important factor on the adsorption of the calcined adsorbent where orange II and methyl orange with negative-charged molecule were eliminated more in comparison with neutral and cationic dye molecules, according to the chemical adsorption due to the electrostatic interaction. The amount of orange II was removed more than that of methyl orange as a result of the structural affinity on reconstruction of layered double hydroxide with host-guest interaction