Metal Phosphonate Metal-Organic Frameworks (MOFs) have recently garnered interest as a possible solution to many issues plaguing modern society including but not limited to sustainable energy, catalysis, climate change, biomedical applications, etc. While previous attempts at synthesizing metal phosphonate MOF species have been successful, the products are microcrystalline and generally exhibit small pore sizes. Additionally, due to the nature of synthesis, metal phosphonate MOFs exhibit significant defect loading into the regular lattice of the synthesized crystal, degrading the material properties of the substance. The goal of this research was to optimize the synthesis of phosphonic acid precursor ligands as well as to explore and optimize phosphonate MOF synthesis in an attempt to open the field up to greater interest from the MOF community. The results were mixed as we report successful optimization and prototyping of more traditional and newly synthesized phosphonic acid ligands but were unsuccessful in optimizing the synthesis of the MOF material. Phosphonic acid ligand synthesis was demonstrated to be versatile and thorough in its substitution, yielding variety of phosphonic acid species. Investigations into the mechanistic progression of MOF synthesis revealed numerous obstacles impending the formation of large, regular lattices that resulted in inconsistent reaction products. While some issues were able to be overcome, certain fundamental aspects of the system such as the denticity of the ligand and the reactivity of the metal constituent were viewed as insurmountable based on current synthetic methodologies.