In this project we target the development of new methodologies to synthesize lithium metal-organic frameworks (MOFs). Even though many transition-metal based MOFs are known, due to the unique chemistry of lithium, very few lithium MOFs have been reported so far, and even fewer are porous. Using lightweight elements such as lithium as building blocks can help decrease the framework density, which can in turn increase gravimetric uptake capacity of gas molecules. Through this study, synthetic strategies that take advantage of phenolate-based heterofunctional ligands specifically tailored for lithium frameworks have been developed and proved to be effective. With these strategies, a number of novel Li-MOFs have been synthesized and structurally characterized. The synthesis, crystal structures, and framework topologies are described, together with select gas sorption properties.