The chemistry presented in this thesis focuses on three projects involving the organometallic chemistry of uranium complexes. The first encompasses attempts to form isolable uranium metallocene phenyl species based on the previously synthesized (C5Me5)2UPh2, which was reported to undergo decomposition to a transient benzyne complex, (C5Me5)2U(C6H4), in solution. Initial attempts to produce the diphenyl complex for study led to the isolation of a new uranium benzyne complex, [(C5Me5)2UPh(μ2¬-C6H4)][Li(Et2O)]. Further studies with the [C5Me4(SiMe3)]− ligand led to the isolation of a metallated phenyl complex, [η5:η1-C5Me4(SiMe2CH2]U(C6H5), that is not a benzyne and [C5Me4(SiMe3)]2UBr(C6H5). The second project focuses on the development of the uranyl moiety, [UO2]2+, as a precursor for organometallic complexes of uranium. This study has led to the isolation of the new uranyl complexes UO2[N(SiMe3)2](NO3)(THF)2, [NEt4][(C5Me5)UO2(NO3)2], and [NEt4]2[UO2(η1-NO3)2(η2-NO3)2]. The third project involves the use of thermal analysis of organouranium compounds to test the viability of uranium nitride production from species dense in nitrogen atoms and to gain a better understanding of the thermal properties of organouranium species.