[en] Reduction of the uranium(III) metallocene [(η${}^5$‐C${}_5^i$Pr${}_5$)${}_2$UI] (1) with potassium graphite produces the “second‐generation” uranocene [(η${}^5$‐C${}_5^i$Pr${}_5$)${}_2$U] (2), which contains uranium in the formal divalent oxidation state. The geometry of 2 is that of a perfectly linear bis(cyclopentadienyl) sandwich complex, with the ground‐state valence electron configuration of uranium(II) revealed by electronic spectroscopy and density functional theory to be 5f${}^3$ 6d${}^1$. Appreciable covalent contributions to the metal‐ligand bonds were determined from a computational study of 2, including participation from the uranium 5f and 6d orbitals. Whereas three unpaired electrons in 2 occupy orbitals with essentially pure 5f character, the fourth electron resides in an orbital defined by strong 7s‐6${}_{x^2}$ mixing. (© 2019 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim)