Laboratory-synthesized nanocarbon pelletized with titanosilicate (ETS-10) as a support matrix has been investigated for the capture of radioactive iodine present as methyl iodide (CH3I) in the off-gas streams produced during aqueous reprocessing of used nuclear fuel. The mass fraction of carbon in the sorbent matrix was 0.10. The effects of residence time and CH3I concentration were investigated using a continuous flow column setup to quantify the adsorption and desorption capacities of adsorbent under dynamic conditions from an air stream containing CH3I present at concentrations representative of those expected in the off-gas streams. Air with CH3I gas as a source in the column resulted in quantifiable CH3I adsorption with 0.98 mg/g of adsorption capacity. Laboratory-made nanocarbons had a larger adsorption capacity than those of the other carbons reported in the literature. Additionally, the adsorption capacity of nanocarbon on ETS-10 is compared to that of nanocarbon coated on cordierite in previous studies.