Uranium recovery has profound significance in both uranium resource acquisition and pollution treatment. In recent years, metal‐organic frameworks (MOFs) have attracted much attention as potential uranium adsorbents owing to their tunable structural topology and designable functionalities. This review explores the research progress in representative classic MOFs (MIL‐101, UiO‐66, ZIF‐8/ZIF‐67) and other advanced MOF‐based materials for efficient uranium extraction in aqueous or seawater environments. The uranium uptake mechanism of the MOF‐based materials is refined, and the structure/functionality‐property relationship is further systematically elucidated. By summarizing the typical functionalization and structure design methods, the performance improvement strategies for MOF‐based adsorbents are emphasized. Finally, the present challenges and potential opportunities are proposed for the breakthrough of high‐performance MOF‐based materials in uranium extraction.