Metal-organic frameworks (MOFs) are crystalline porous materials with excellent gas storage capacities and unique chemical tunability. Their application as new materials to uptake and degrade chemical warfare agents has been the topic of intense study over the last half-decade. Work by others proved that Zr-MOFs and polymer composites made from them are contenders for the next generation of personal protective equipment (PPE) for combatting nerve agents. In an attempt to speed up discovery and understanding of MOF catalysts for nerve agent degradation, a high-throughput screening (HTS) assay was developed for a common nerve agent simulant. Chapter 2 outlines the development of this assay as well as the curation and screening results from the library of 93 MOFs and related materials. Successful development and validation of the HTS assay led to targeted attempts to apply this method for both a wider array of MOFs as well as MOF-polymer composites. Chapter 3 uses the speed of HTS to investigate two groups of closely related MOFs that result in a wide range of catalytic activities. This chapter also adapts the HTS assay to analyze composites and again finds that small differences in materials changes the outcome of catalyst performance. Chapter 4 describes the development of a new HTS assay with another nerve agent simulant that can be directly compared to results of the assay developed in Chapter 2. This new assay expands understanding of the degradation attempts by MOF catalysts to date. In addition, this new HTS method was compared to a medium-throughput method for monitoring breakdown of nerve agent VX and was confirmed by literature assay using 31P NMR. MOF catalysts design was paired with MOF-polymer composite design, when a new strong, ductile hybrid was developed in Chapter 5. Catalytically active MOFs were combined with a spandex polymer to target composites for durable PPE. The HTS assay was used to show catalytic ability of these composites and three processing methods demonstrated the versatility of these MOF-polymer composites.