Recent research has demonstrated the degradation of organophosphonates through hydrolysis using microporous UiO–66–NH2‐fabric composites. Yet, challenges remain due to the limitations of organophosphonates accessing active sites in large, engineered granules. To address this, an innovative approach to integrate mesoporous UiO–66–NH2 onto various fabrics is provided, thereby overcoming previous mass transfer limitations. Mesoporosity in the UiO–66–NH2‐fabric is attributed to the amphoteric cocamidopropylbetaine (CAPB) surfactant which templates the mesochannel construction. Unexpectedly, because the synthesis is aqueous, benign, low temperature (60°C), and avoids strong acids and toxic solvents, it is compatible with fragile supports such as untreated cotton. The UiO–66–NH2‐fabric composite formed using treated polypropylene (PP) attains a BET specific surface area of 360 m2 g−1comp. Remarkably, the mesoporous UiO–66–NH2‐composites exhibit a pore volume as large as 0.2 cm3 g−1comp, 33% in the mesoporous range, which is higher than other previous reports. Practically, the mesoporous UiO–66–NH2‐treated PP composite enhances the rate of methyl paraoxon (DMNP) degradation, showing a t1/2 value that is 15 times faster than microporous UiO–66–NH2 composites measured under the same conditions. Similar trends are observed in the degradation of actual nerve agents. These composites hold significant potential across diverse applications, including filtration, protection, and catalysis.