ETS-10 supported hollow carbon nanostructured polyhedron adsorbent, C@ETS-10, was synthesized by wet impregnation method to evaluate removal of iodine from off-gas stream from a used nuclear fuel reprocessing operation. The characteristics of the adsorbent were investigated by various techniques such as transmission electron microscopy (TEM), scanning electron microscopy-energy dispersive spectroscopy (SEM-EDS), powder X-ray diffraction (P-XRD) and thermogravimetric analysis (TGA), revealing uniform hollow carbon nanostructured polyhedrons with particle size 10-30 nm supported onto ETS-10. The total BET surface area of 10 wt% C@ETS-10 adsorbent was 149 m(2) g(-1). The performance of C@ETS-10 nanostructured adsorbent for capture of volatile iodine from gas stream was determined as a function of parameters such as the carbon loading, operating temperatures and empty bed contact time (EBCT). Observed sorption capacity of adsorbent was 28.9 mg g(-1) of volatile iodine at 20 degrees C without any chemical reaction with sorbent. The maximum dynamic capacity of a column of 10 wt% C@ETS-10 was calculated to be 40 mg g(-1). The nanostructured adsorbent has potential to capture environmental impact of radionuclide off-gas emission from nuclear industry. (C) 2015 Elsevier B.V. All rights reserved.