Hydrothermal synthetic methods have been utilized to synthesize many compounds containing both uranium and transition metals, as well as hybrid organic-inorganic materials. These compounds are found to adopt zero-, one-, two- and three-dimensional structural typologies. Of the 22 compounds covered in this dissertation, seven (31.8%) are based upon sheets of polyhedra, two (9.1%) are based upon chains of polyhedra, and three (13.6%) are based upon limited cluster polyhedra. There are ten (45.5%) structures based upon three-dimensional frameworks. Single crystal diffraction experiments reveal that the seven sheet structures contain transition metal cations (Ag⁺, Co ²⁺, Mn²⁺, Cu²⁺). The ten three-dimensional frameworks contain transition metal substructures (Ag⁺, Hg ²⁺, Ni²⁺, Co²⁺, Zn²⁺), metal-organic framework (MOF) structures and porous low-valence uranium framework.

There are two chain structures containing bimetallic metal-organic hybrids and single metal-organic hybrids. Three limited polyhedra structures contain mononuclear and binuclear clusters are also described. All structures were determined through the use of single crystal X-ray diffraction with the aid of EDAX and X-ray powder diffraction analysis. Addition characterization includes Raman spectroscopy, fluorescent spectroscopy, ion-exchange, and thermal stability.