Radioactive iodine isotopes that are produced in nuclear power plants and used in medical research institutes could be a serious threat to the health of many people if accidentally released to the environment because the thyroid gland can absorb and concentrate them from a liquid. For this reason, uptake of iodide anions was investigated on microrosette-like d-Bi2O3 (MR-d-Bi2O3). The MR-d-Bi2O3 adsorbent showed a very high uptake capacity of 1.44 mmol g-1 by forming insoluble Bi4I2O5 phase. The MR-d-Bi2O3 also displayed fast uptake kinetics and could be easily separated from a liquid after use because of its novel morphology. In addition, the adsorbent showed excellent selectivity for I- anions in the presence of large concentrations of competitive anions such as Cl- and CO32-, and could work in a wide pH range of 4-11. This study led to a new and highly efficient Bi-based adsorbent for iodide capture from solutions.