In order to enhance the adsorption capacity of hydrotalcite material for heavy metal ions, the LDH/CMC composite was prepared by a simple hydrothermal method. The XRD pattern showed that the presence of CMC has no obvious influence on the crystal structure of hydrotalcites. The FT-IR and UV-vis DRS analyses showed that the CMC functionalized surface has been obtained. The SEM and BET/BJH showed that the morphologies, textural and surface chemical properties of LDH were affected remarkably after the introduction of CMC. The weight percentage of CMC in the LDH/CMC composite was estimated to be about 17.4%. The adsorption experiments showed the LDH/CMC composite exhibited high efficiency in the Cu(II) removal at pH > 6.5, affording Cu(II) removal rates of 92.3%. The results demonstrated that the LDH/CMC composite was a suitable adsorbent for Cu(II)-contaminated wastewater treatment.