Green rust (GR), a layered double hydroxide (LDH) containing Fe, and magnetite can be found in natural and engineered environments. The ability of chloride GR (GR-Cl) and magnetite to retain iodide as a function of various parameters was investigated. Sorption equilibrium is achieved within 1 day of contact time between iodide and preformed GR-Cl in suspension. pHm variations (7.5-8.5) have no significant influence, but the iodide sorption decreases with increasing ionic strength set by NaCl. Sorption isotherms of iodide suggest that the uptake operates via ionic exchange (IC), which is supported by geochemical modeling. The short-range binding environment of iodide associated with GR is comparable to that of hydrated aqueous iodide ions in solution and is not affected by pHm or ionic strength. This finding hints at an electrostatic interaction with the Fe octahedral sheet, consistent with weak binding of charge balancing anions within an LDH interlayer. The presence of sulfate anions in significant amounts inhibits the iodide uptake due to recrystallization to a different crystal structure. Finally, the transformation of iodide-bearing GR-Cl into magnetite and ferrous hydroxide resulted in a quantitative release of iodide into the aqueous phase, suggesting that neither transformation product has an affinity for this anionic species.