The nature of actinide-actinide bonds has attracted considerable attention for a long time, especially since recent theoretical studies suggest that triple and up to quintuple bonds should be possible, but little is known experimentally. Actinide-actinide bonds inside fullerene cages have also been proposed, but their existence has been debated intensively by theoreticians. Despite all the theoretical arguments, critical experimental data for a dimetallic actinide endohedral fullerene have never been obtained. Herein, we report the synthesis and isolation of a dimetallic actinide endohedral metallofullerene (EMF), U-2@C-80. This compound was fully characterized by mass spectrometry, single crystal X-ray crystallography, UV-vis-NIR spectroscopy, Raman spectroscopy, cyclic voltammetry, and X-ray absorption spectroscopy (XAS). The single crystal X-ray crystallographic analysis unambiguously assigned the molecular structure to U-2@I-h(7)-C-80. In particular, the crystallographic data revealed that the U-U distance is within the range of 3.46-3.79 A, which is shorter than the 3.9 angstrom previously predicted for an elongated weak U-U bond inside the C-80 cage. The XAS results reveal that the formal charge of the U atoms trapped inside the fullerene cage is +3, which agrees with the computational and crystallographic studies that assign a hexaanionic carbon cage, (I-h-C-80)(6-). Theoretical studies confirm the presence of a U-U bonding interaction and suggest that the weak U-U bond in U-2@I-h(7)-C-80 is strengthened upon reduction and weakened upon oxidation. The comprehensive characterization of U-2@I-h(7)-C-80 and the overall agreement between the experimental data and theoretical investigations provide experimental proof and deeper understanding for actinide metal-metal bonding interactions inside a fullerene cage.