A new type of double uranium oxo cation [O-U-O-U-O]4+ is prepared by selective oxygen-atom abstraction from macrocyclic uranyl complexes using either boranes or silanes. A significant degree of multiple U[double bond, length as m-dash]O bonding is evident throughout the U2O3 core, but either trans-,cis- or trans-,trans-OUOUO motifs can be isolated as boron- or silicon-capped oxo complexes. Further controlled deoxygenation of the borylated system is also possible.