This account highlights recent research from our laboratory on nonaqueous plutonium coordination chemistry. The preparation of organic-soluble synthons, the reactivity of plutonium with soft donor atom ligands, and initial characterization of resultant complexes are presented. Homoleptic soft donor complexes are targeted, to contrast with the much larger body of actinide chemistry that focuses covalency and reactivity within one to three sites in the coordination sphere. Structural parameters from X-ray structure determination and computation indicate small, yet significant, differences in covalency between isostructural plutonium and lanthanide complexes. Results are discussed in the context of our aim to expand the fundamental chemistry of plutonium, particularly to address challenges in the nuclear industry.