There is a critical need for novel composite materials for high-performance chemical filtration and detoxification of organophosphonates (OPs) and other harmful compounds found in nerve agents, pesticides, and industrial processes. In this work, rapid hydrolysis of OPs using high-surface-area zirconium-based MOF-aerogel composites is demonstrated. Using a unique surfactant-templated solvothermal synthesis method, mesoporous UiO-66-NH