Novel heterobimetallic complexes featuring a uranium atom paired with a first-row transition metal have been computationally predicted and analyzed using density functional theory and multireference wave function based methods. The synthetically inspired metalloligands U{((Pr2PCH2NAr)-Pr-i)(3)tacn} (1) and U((Pr2PCH2NPh)-Pr-i)(3) (2) are explored in this study. We report the presence of multiple bonds between uranium and chromium, uranium and manganese, and uranium and iron. The calculations predict a 5-fold bonding between uranium and manganese in the UMn((Pr2PCH2NPh)-Pr-i)(3) complex, which is unprecedented in the literature.