The carbamoylmethylphosphine oxide (CMPO) functionalized MIL-101(Cr) was investigated as a potential uranium scavenger. This metal-organic framework-based adsorbent shows very high selectivity toward uranium, as well as thorium, in competition with various rare earth metals. Furthermore, it showed rapid adsorption kinetics, in both batch conditions and a dynamic (column) setup. The adsorbent is fully regenerable, using oxalate solution. Fast elution kinetics in the column setup were observed during the regeneration. In addition, reusability studies were performed under dynamic conditions. Five consecutive adsorption/desorption cycles were carried out, showing a consistent 100% recovery, at pH 4, using 0.1 M oxalate solution as an effective stripping agent. Additionally, the successive use over various adsorption/desorption cycles with constant performance proves the high stability of this adsorbent in an acidic, aqueous environment.