The β-cyclodextrin/Al(OH) 3 composites (β-CD/Al(OH) 3 ) were synthesized using the plasma-induced grafting technique and were employed to remove UO 2 2+ from aqueous solutions under ambient conditions. Based on the characteristic results of SEM, FT-IR, XRD, and TGA techniques, β-CD was satisfactorily grafted onto the Al(OH) 3 surface. The maximum adsorption capacity of β-CD/Al(OH) 3 composites calculated from Langmuir model at pH6.0 and 303K was 63.29mg/g, which was significantly higher than Al(OH) 3 (23.31mg/g). The high adsorption capacity of β-CD@Al(OH) 3 composites was due to the inner cores of the hydrophobic cavity of CD incorporated with UO 2 2+ ions. The calculated thermodynamic parameters showed that the adsorption of UO 2 2+ on Al(OH) 3 and β-CD@Al(OH) 3 composites was an endothermic and spontaneous process. The batch desorption indicated that the adsorption of UO 2 2+ on β-CD@Al(OH) 3 composites was an irreversible process. Based on the surface complexation modeling, the adsorption mechanism of UO 2 2+ on Al(OH) 3 and β-CD@Al(OH) 3 composites was outer-sphere surface complexation at pH<5.0, whereas inner-sphere surface complexation dominated the UO 2 2+ adsorption on Al(OH) 3 and β-CD@Al(OH) 3 composites at pH>6.0. These observation showed that β-CD/Al(OH) 3 composite can be used as a promising adsorbent for the preconcentration and immobilization of UO 2 2+ ions in environmental pollution cleanup.