This article states the first application of nickel/molybdenum-layered double hydroxide (LDH) as a new adsorbent for the removal of cadmium ions [Cd(II)] from aqueous solutions. The essential structure of Ni/Mo-LDH of di and hexavalent cations was elucidated by X-ray photoelectron spectroscopy, X-ray diffraction, and Fourier transmission infrared spectroscopy. The maximum adsorption capacity of adsorbent is 53.6 mgg(-1) at a temperature of 298K, pH of 5.5, mass of 0.5gL(-1), time of 105min, and initial concentration of 175 mgL(-1). This adsorbent was distinguished by self and fast separation from adsorption media due to its layered, mesoporous structure and the presence of hexavalent molybdenum cation.