We report the synthesis and spectroscopy of pseudo-halide complexes of uranyl coordinated to salicylaldiminate ligands. The reaction of [(NC9H6)N=C(H)C6H2tBu2O-κ3(O,N,N′)]UO2Cl(THF), 1, with NaN3 produces a rare example of an uranyl azide, [(NC9H6)N=C(H)C6H2tBu2O-κ3(O,N,N′)]UO2(N3)(THF), 2. A series of isocyanates, [(NC9H6)N=C(H)C6H2tBu2O-κ3(O,N,N′)]UO2(NCE)(THF), E = O, 3; S, 4; Se, 5, were synthesized from reaction of 1 with KNCE. Reaction of 1 with AgNO3 and AgOTf (OTf = SO3CF3) produces [(NC9H6)N=C(H)C6H2tBu2O-κ3(O,N,N′)]UO2(NO3), 6 and [(NC9H6)N=C(H)C6H2tBu2O-κ3(O,N,N′)]UO2(OTf)(THF), 7, respectively. The newly formed complexes, 2–7, have been characterized by 1H, 13C, and 15N NMR (where applicable), as well as IR spectroscopy, and the molecular structure of 2, 5, 6, and 7 have been determined by X-ray crystallography.