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The novel ion-imprinted montmorillonite nanosheets/chitosan (IIMNC) gel beads were prepared for selective adsorption of Cu2+. The IIMNC gel beads were characterized by scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FTIR), and X-ray photoelectron spectroscopy (XPS). The results showed that IIMNC was successfully assembled and rich in honeycombed pores, which performed well in the removal of Cu2+ through the synergistic effect of montmorillonite nanosheets and chitosan. The elimination of copper was followed by