Radioactive iodine anion wastewater is generated during the operation of nuclear facilities. Efficiently adsorbing and removing radioactive iodine is crucial for the sustainable development of nuclear energy. A potential adsorbent, nano silver-loaded activated carbon fiber (Ag@ACF), was prepared through hydrothermal synthesis and high-temperature vacuum reduction for the efficient removal of iodide anions. The as-prepared Ag@ACF composite has been comprehensively characterized, with silver nanoparticles uniformly distributed on the surface and pore walls of the Ag@ACF, enhancing the adsorption sites for iodine anions. The adsorption performance of Ag@ACF towards iodine anions was evaluated through column and batch experiments, varying silver concentration, adsorbent dosage, pH, contact time, and competing anions. Ag@ACF demonstrated high water stability and a low desorption rate of iodine anions. At a pH of 2, Ag@ACF exhibited a maximum adsorption capacity for iodine anions of 372 mg/g, surpassing most other adsorbents and showing promise for engineering applications. Adsorption kinetics and isotherm analysis indicated that the adsorption process of Ag@ACF primarily involved monolayer homogeneous chemisorption, resulting in the formation of stable AgI. These results suggest that Ag@ACF could serve as a potential adsorbent for removing iodine from radioactive wastewater.