Natural green rust (GR) can retard the migration of anions through geological media because it has a Layer Double Hydroxyl (LDH) structure with a positive charge. In this study, the sorption behaviors of anions such as selenite (<TEX>$Se(IV)O{_3}^{2-}$</TEX>), selenate (<TEX>$Se(VI)O{_4}^{2-}$</TEX>), and iodide (<TEX>$I^-$</TEX>) onto green rusts with different structures, i.e., GR(<TEX>$Cl^-$</TEX>) and GR(<TEX>$CO{_3}^{2-}$</TEX>), were investigated by conducting batch sorption experiments in an anoxic condition. Experimental results showed that selenite was mostly sorbed onto GR(<TEX>$CO{_3}^{2-}$</TEX>) and then partly reduced to metal selenium, Se(0). However, little selenate and iodide was sorbed onto GR(<TEX>$CO{_3}^{2-}$</TEX>) while some iodide was sorbed onto GR(<TEX>$Cl^-$</TEX>). It is presumed from the experimental results that the major sorption mechanism of <TEX>$SeO{_3}^{2-}$</TEX> and <TEX>$I^-$</TEX> onto green rusts is the anion exchange reaction with the anions existing in the interlayer of the rusts. Green rust, therefore, can play an important role in the retardation of anions migrating through deep geological environments owing to its LDH structure with a high anion exchange capacity.