Fluorinated and chlorinated molecules represent >30% of active pharmaceuticals and >40% of agrochemicals due to their improved metabolic stabilities and lipophilicities compared to their non-halogenated analogues. However, the selective installation of these elements is challenging due to the uncontrollable reactivity of halogenating molecules, which are often toxic gasses or prohibitively unstable reagents. Therefore, the bulk of my graduate research has focused on the development of novel materials for the safe handling of the halogens, imparting tunable synthetic control and thus “taming” their reactivity. These materials, metal-organic frameworks (MOFs), are porous, crystalline, insoluble solids constructed from organic linkers and inorganic nodes. Their tunable structures at both their metal secondary building unit (SBU) and organic linkers impart MOFs with inherent utility, allowing for tunable host-guest interactions such as gas capture and catalysis. Larger (> 10 Å) pore MOFs facilitate diffusion of substrates throughout the material, and the insoluble nature of MOFs begets advantages implicit to heterogeneous materials when considering catalytic utility. Using MOFs to sequester dangerous gasses is well-established in the literature, but few examples employ MOFs as heterogenous catalysts in tandem with toxic gas/reagent delivery. My graduate research has focused on the synthesis of MOFs that are unique in their ability to not only retain crucial material properties after exposure to elemental halogens, but also deliver the sequestered halogen to a synthetic target and drive the catalytic halogenation of a range of organic molecules. Additionally, I have devised a novel strategy for the solvent-free preparation of these MOFs on scale, alleviating the use of toxic solvents and shortening the synthesis time from 17 days to 1 day.