Proliferation of nuclear technology has also resulted in radionuclide release into the environment. Key among them is radioiodine which threatens human health through thyroid cancer and endangers the environment. The efficient removal of iodine is important to curb these threats. Herein we report a facile in situ Cu-ZnO decorated JUC-160 derived carbon for efficient volatile iodine adsorption. The as-prepared Cu/ZnO@C displayed a high iodine adsorption capacity of 521 wt% and 1280.14 mg g−1 in vapor phase and in solution respectively. Furthermore, kinetics and isotherm studies showed a monolayer and chemisorption dominant adsorption process confirmed by pseudo-second-order and Langmuir models. Moreover, this high adsorption capacity and mechanism was attributable to electron-donor-acceptor interactions, charge transfer complexes and oxidation of Cu0 to Cu+. Additionally, the in situ doping of nitrogen via the ligands used resulted in added nitrogen sites for iodine immobilization. The as-fabricated material also exhibited exceptional recovery and reusability such that it is proposed as a promising volatile iodine adsorbent.