The Ni(II)Fe(III)-LDO has been synthesized by calcination of Ni(II)Fe(III)-LDH at 500 ℃. The prepared LDO is applied in the treatment of Methyl Orange (MO) dye from a synthetic solution. A batch of experiments is conducted to examine the effects of varying adsorption parameters, i.e. initial dye concentrations and temperature. The results indicate that the adsorption of MO increases with rising dye concentration and solution temperature. Temkin, Freundlich, and Langmuir isotherms are analyzed to investigate the adsorption process at different pH levels. Various thermodynamic parameters such as ΔS, ΔH and ΔGº have also been calculated. The adsorption of MO dyes on the Ni(II)Fe(III)-LDO is found endothermic and non-spontaneous in nature. The findings reveal the adsorption process is physical sorption.