Quantum chemical calculations suggest that a series of molecules with the general formula MAu4 are stable, where M = U, Th, and a group-4 atom. They correspond to Au in the formal valence state −1 and indicate that gold can act as a ligand similar to the halogen series. Of the MAu4 species studied, UAu4, the first predicted mixed gold uranium compound, has a short M−Au bond distance, 2.71 Å, which would locate Au between Br and I from the bond length point of view in the U-tetrahalide series. Energetically, the U−Au bond is weaker than the corresponding U−Br and U−I bonds.