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Efficient and cost-effective removal of radioactive iodine anions from contaminated water has become a crucial task and a great challenge for waste treatment and environmental remediation. Herein, we present hexadecylpyridinium chloride monohydrate modified bentonite (HDPy-bent) for the efficient and selective removal of iodine anions (I− and IO 3 −) from contaminated water. Batch experiments showed that HDPy-bent could remove more than 95% of I− and IO 3 − within 10 min, and had maximum I− and IO 3 − adsorption capacities of 80.0 and 50.2 mg/g, respectively. Competitive experiments indicated that HDPy-bent exhibited excellent I− and IO 3 − selectivity in the excessive presence of common concomitant anions including PO 4 3−, SO 4 2−, HCO 3 −, NO 3 −, Cl− (maximum mole ratio of anions vs iodine anions was ∼50,000). An anion exchange mechanism was proposed for the selective adsorption of iodine anions. Optimal adsorption structure of HDPy+/I− (IO 3 −) at atomic level and driving forces of the I− (IO 3 −) adsorption were calculated by density functional theory (DFT) simulations. Moreover, the good durability and reusability of the HDPy-bent has been demonstrated with 5 adsorption-desorption cycles. Dynamic column experiment also demonstrated that HDPy-bent exhibited excellent removal and fractional recovery capabilities towards I− and IO 3 − from simulated groundwater and environmental water samples. In conclusion, this work presents a promising adsorbent material for the decontamination of radioactive iodine anions from wastewater on a large scale. [Display omitted] • HDPy-bent showed excellent adsorption abilities for iodide and iodate. • Anions exchange mechanism was confirmed by batch experiments and DFT simulations. • The pyridine N was the intrinsic active site of the modified bentonite. • HDPy-bent was efficient for removing radioiodine anions from wastewater. [ABSTRACT FROM AUTHOR]