This cover picture depicts a 3‐hydroxy‐2‐pyridinone (3,2‐HOPO) functionalized nano‐MOF, MIL‐101‐HOPO, as an in vivo decorporation agent to remove uranyl in mice. With the increasingly widespread application of uranium in nuclear industry, the potential nuclear accidents and nuclear contamination have led to widespread concern on how to reduce the damage of uranyl toward living organisms. By combining the excellent actinide chelating ligand 3,2‐HOPO and the mesoporous cage nano‐MOF MIL‐101, we have effectively demonstrated the improved adsorption efficiency, adsorption selectivity and in vivo sequestration efficacy of MIL‐101‐HOPO toward uranyl compared with the pristine nano‐MOFs, revealing the promising application of functionalized nano‐MOFs in the field of actinide decorporation. More details are given in the article by Diwu et al. on page 2054—2060.