The work presented in this dissertation is primarily focused on the synthesis and characterization of thorium and uranium containing coordination polymers using benzenediphosphonate and carboxyphenylphosphonate derivatives as ligands. I investigated three broad areas of study that determined the structural features and properties of these materials as they apply to sequestration and remediation of actinide waste and their potential material applications.  The first area of investigation is concerned with the use of structure directing agents in the assembly of uranyl diphosphonate frameworks. This work which began with simple templates such as organoammonium cations, was later extended to encapsulated cations, hydronium- and alkali metal-crown ether inclusion complexes, and was concluded using alkali metal ions. Two elliptical uranyl nanotubules were isolated along with other series of framework materials with voids that are filled with alkali metal cations and organic templates respectively. I developed the first highly stable functional uranyl nanotubule with exceptional ion-exchange properties towards monovalent cations. The second area of research explores the structural features and trends in actinide diphosphonates and carboxyphosphonates as important tools in understanding how actinides behave in the biological and geological environments. The dimensionality and overall topology of these compounds depends on the coordination preferences of the metals as well as the functionalized organic ligands. The rigid phenyl spacer connects low-dimensional uranyl chains into layered three-dimensional pillared structures. Uranyl cations display a high propensity for phosphonates over the carboxylate moieties of the bifunctional ligands examined in agreement with the hard-soft acid-base prediction.  In the final part of the dissertation I utilized the hard-soft acid-base distinctions to prepare heterometallic uranyl-transition metal coordination polymers using carboxyphenylphosphonate ligands. The objective was to develop actinide materials for magnetic or other material applications. I demonstrated the importance of using pliable 1,2-carboxyphenylphosphonate ligand in stabilizing high nuclearity uranyl heteropolyoxometalate cage clusters under mild hydrothermal condition. This work suggests that metal linkers are needed to complete the sphere. In addition, this result opens up this field for exploration as this material represents an excellent model system with which to design and study uranyl nanoclusters. Moreover, this research will undoubtedly stimulate much more activity in this important area of actinide chemistry in the future.