Uranium containing clusters UnOm and complexes U+(N2)n are produced in a molecular beam via laser vaporization in a pulsed supersonic expansion. Mass-selected cations are investigated using fixed frequency photodissociation with 355 and 532 nm Nd:YAG harmonics. The most stable structures and stoichiometries are formed as fragment ions during photodissociation. Infrared photodissociation spectra of U+(N2)n are measured with a tunable infrared OPO/OPA. Density functional theory is used to investigate those masses found to be most stable. Computational predictions of infrared spectra are compared to experimental data. Uranium oxide clusters were found to fragment to UO2+(UO3)n regardless of the identity of the ion photodissociated. Additional fragment cations (UO3)n+ are produced only from cluster cations (UO3)n+ indicate the stability of the neutral (UO3)n cluster or n(UO3) eliminated. The complex U+(N2)8 was found to be a fully coordinated cube. Photodissociation of U+(N2)n with 355 and 532 nm light produced a regular ratio of photon energy to the number of ligands eliminated. This was used to estimate a U+-N2 bond dissociation energy of 12.1 ± 1.3 kcal/mol, which was found not to vary significantly with complex size. DFT calculations are in good agreement with this bond energy, and were able to accurately predict infrared spectra of U+(N2)8 and other fully coordinated uranium cation complexes. However, agreement between experiment and theory was found to become poorer as complex size is reduced from n = 8 to 3.