Iodine-129 poses a significant challenge in the drive towards lowering radionuclide emissions from used nuclear fuel recycling operations. Various techniques are employed for capture of gaseous iodine species, but it is also present, mainly as iodide anions, in problematic residual aqueous wastestreams, which have stimulated research interest in technologies for adsorption and retention of the radioiodine. This removal effort requires specialised adsorbents, which use soft metals to create selectivity in the challenging chemical conditions. A review of the literature, at laboratory scale, reveals a number of organic, inorganic and hybrid adsorbent matrices have been investigated for this purpose. They are functionalised principally by Ag metal, but also Bi, Cu and Pb, using numerous synthetic strategies. The iodide capacity of the adsorbents varies from 13 to 430 mg g−1, with ion-exchange resins and titanates displaying the highest maximum uptakes. Kinetics of adsorption are often slow, requiring several days to reach equilibrium, although some ligated metal ion and metal nanoparticle systems can equilibrate in < 1 h. Ag-loaded materials generally exhibit superior selectivity for iodide verses other common anions, but more consideration is required of how these materials would function successfully in industrial operation; specifically their performance in dynamic column experiments and stability of the bound radioiodine in the conversion to final wasteform and subsequent geological storage.