Among the numerous nuclear wastes, radioactive iodine (I-2) has become one of the main pollutants due to its serious adverse effects on the human thyroid gland. Therefore, the design and synthesis of adsorbents for efficient elimination of radioactive I-2 from nuclear waste is an attractive target. Herein, we developed a novel silver nanoparticle (AgNP)-loaded metal-organic framework (MOF) of UiO-66, which exhibits excellent I-2 adsorption performance due to the synergistic effect between UiO-66 MOFs and AgNPs. The designed AgNPs@UiO-66 adsorbent possesses good porosity and high Ag-loading ability, which assists the adsorbent to achieve a high adsorption I-2 capacity of 1260 mg/g. The pseudo-second-order model and Langmuir model are considered to be suitable for describing the I-2 adsorption behavior over AgNPs@UiO-66. Additionally, some important experimental parameters, such as adsorption time, adsorbent concentration, secondary pollution, and adsorption mechanism, have also been studied in detail. These satisfactory results manifest that AgNPs@UiO-66 is a latent adsorbent for I-2 removal in nuclear waste management.