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The nuclear fuel cycle inevitably generates a large amount of radioactive waste liquid,which will pose a serious threat to the ecological environment and human health.Ion exchange method has received wide attention for its easy operation,low cost and no secondary pollution.However,the effective removal of radioactive ions from complex solutions still remains a serious challenge due to their environmental mobility and radiotoxicity.We have developed an effiicient strategy to construct crystalline ion-exchange materials by inducing layered or three-dimensional microporous anionic frameworks by organic cations that can be effectively exchanged by radioactive metal ions.This type of materials can be applied effectively to the removal of radioactive ions from complex solutions and the removal mechanism has been deeply clarified by means of single crystal structure analyses,theoretical calculations,etc.This review summarizes our recent progress in the study of synthesis,structures and properties of radioactive ion removals for such type of crystalline ion-exchange materials.