Four new uranium–ruthenium complexes, [(TrenTMS)URu(η5‐C5H5)(CO)2] (9), [(TrenDMSB)URu(η5‐C5H5)(CO)2] (10), [(TsTolyl)(THF)URu(η5‐C5H5)(CO)2] (11), and [(TsXylyl)(THF)URu(η5‐C5H5)(CO)2] (12) [TrenTMS=N(CH2CH2NSiMe3)3; TrenDMSB=N(CH2CH2NSiMe2tBu)3]; TsTolyl=HC(SiMe2NC6H4‐4‐Me)3; TsXylyl=HC(SiMe2NC6H3‐3,5‐Me2)3], were prepared by a salt‐elimination strategy. Structural, spectroscopic, and computational analyses of 9–12 shows: i) the formation of unsupported uranium–ruthenium bonds with no isocarbonyl linkages in the solid state; ii) ruthenium–carbonyl backbonding in the [Ru(η5‐C5H5)(CO)2]− ions that is tempered by polarization of charge within the ruthenium fragments towards uranium; iii) closed‐shell uranium–ruthenium interactions that can be classified as predominantly ionic with little covalent character. Comparison of the calculated URu bond interaction energies (BIEs) of 9–12 with the BIE of [(η5‐C5H5)3URu(η5‐C5H5)(CO)2], for which an experimentally determined URu bond disruption enthalpy (BDE) has been reported, suggests BDEs of approximately 150 kJ mol−1 for 9–12.