Effective capture of radioactiveiodine is of paramount importance for the safe and long-term storage of fission products in the nuclear fuel cycle. Herein, as eries of functionalized Th-UiO-66 MOFs wase mployed as a model to investigate the effects of substituents on iodine adsorption in both solution and vapor states. Sorption studies revealed that the electro-donating amino group exhibits the most positive role on increasing the removal rate of iodine from cyclohexane and the uptake capacity of iodine vapor.P articularly,t he disubstituted Th-UiO-66-(NH 2) 2 can effectively remove 91.9 %o fi odine (300 mg L À1) from cyclohexane and capture 969 mg g À1 iodine vapor, significantly highert han 59.6 %a nd 334 mg g À1 of untagged Th-UiO-66,r espectively.I na ddition, the substituent effect on the radiolytic stability of MOFs was for the first time investigated, leadingt ot he unearthing of one of the most radioresistant MOFs Th-UiO-66-NH 2 reportedt od ate.