In this work, Au/ZnAl-layer double oxides (LDO) nanocomposties were prepared through a facile calcination process of AuCl 4 − intercalated ZnAl-layered double hydroxides (LDHs) nanocomposites. The morphology and crystal structure of these nanocomposites were characterized by Scanning electron microscopy (SEM), transmission electron microscopy (TEM), powder X-ray diffraction (XRD), and N 2 sorption analysis. By tailoring the process parameter, such as calcination temperature, heating time and the component composition, the adsorption properties of methyl orange (MO) on the Au/ZnAl-LDO nanocomposites were investigated in this work. In a typical adsorption process, it was found that 0.985mg of MO (0.01gL −1 , 100mL, 1mg of MO in total) can be removed in 60min by utilizing only 2.5mg of Au/ZnAl-LDO (Au content, 1%) as adsorbents. Our adsorption data obtained from the Langmuir model also gave good values of the determination coefficient, and the saturated adsorption capacity of Au/ZnAl-LDO nanocomposites for MO was found to be 627.51mg/g under ambient condition (e.g., room temperature, 1atm). In principle, these hybrid nanostructures with higher adsorption abilities could be very promising adsorbents for wastewater treatment.