“…In recent years, coordination chemistry of actinide elements has gained widespread attention due to their underexplored coordination properties as well as interesting redox and catalytic properties. − Importantly, studies on actinide chemistry mostly focus on uranyl U(VI)O 2 2+ , with significantly fewer studies for any other actinide or oxidation state. − Nowadays, efforts are underway to synthesize and isolate highly reactive low-valent actinide compounds, after the realization of their potential in small-molecule activation and catalysis. ,− Meanwhile, the low-valent actinide complexes are dominated by cyclopentadienyl and related ligands, emphasizing a demand to design and synthesize other organic ligand(s) to stabilize low-valent actinide complexes. ,,, In this context, di- and monoanionic Schiff base ligands are frequently explored due to the presence of a strongly coordinating aryl-oxide donor along with a chelating motif. While multiple U(VI)O 2 2+ , U(IV), and Th(IV) and fewer Np(IV) complexes have been reported with dianionic Schiff base ligands, e.g., of salen type, ,,− uranium complexes with Schiff base ligands have been shown to promote interesting electrochemical processes owing to the noninnocent redox behavior of the ligand(s). − Therefore, there is a need for the in-depth characterization of structure, bond properties, and redox behavior of actinide complexes with nonredox innocent ligands to achieve actinide complexes of desired properties.…”