[en] The chemistry of complexes of the d-transition elements containing organoimido functional groups constitutes a rapidly expanding area of research. Examples of molecules containing multiple terminal imido functional groups now exist for representative elements from groups 5-8. In contrast, f-metal terminal organoimido complexes are still relatively rare, and examples of single actinide metal sites coordinated by greater than one imido ligand are unknown. On the basis of the stability of uranyl ion (UO₂)²⁺, there appears to be no reason why the isoelectronic bis(organoimido) species should not be accessible. Development of this chemistry has been hampered by the lack of synthetic routes to high-valent (V,VI) uranium complexes and by the relatively small number of ligands which have been demonstrated to stabilize these oxidation states. Here we describe the synthesis and structural characterization of the first bis(organoimido) complex of uranium(VI). This species also represents the first complex of uranium(VI) supporting metal-carbon bonding in either a σ- or π-fashion. As part of our studies of preparative routes to uranium organoimido complexes, we are examining generation of uranium imido functionalities by abstraction of an amido hydrogen by a leaving hydrocarbyl or amido ligand. 4 refs., 1 fig