In this work, Ag/X and Ag/Y faujasite zeolites were evaluated as candidate sorbents for the retention of methyl iodide under conditions close to those expected in a severe nuclear accident. Different categories of tests were conducted from laboratory to semi-pilot scales. First, the effects of temperature and water vapour on the CH3I retention/decomposition mechanism were investigated under lab-scale conditions. More specifically, the CH3I adsorption capacities and the fate of its main decomposition products (oxygenated compounds and alkanes) were measured under dynamic conditions at different temperatures (35, 100 and 250 °C). Then, the decontamination factors of Ag/X and Ag/Y silver faujasites exchanged with different silver contents were monitored according to the time on stream using a very low CH3I concentration (1 ppmv). Finally, a parametric study was conducted at semi-pilot scale using realistic [CH3I]/[H2O] molar ratio ≈ 10−6 and temperatures in the range 20–90 °C. Those experiments were helpful in order to assess the effects of some important parameters relevant to the adsorbents or operating conditions.