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This paper describes the scalable fabrication of smart electronic textiles (e-textiles) capable of simultaneous sensing, filtration, and detoxification of sulfur dioxide (SO2). The templated method converts pre-deposited copper metal into copper hydroxide, followed by conversion into a copper-based hexahydroxytriphenylene metal-organic framework (MOF) (Cu3(HHTP)2), to afford a large-area (10 × 10 cm2) conductive coating (sheet resistance = 0.1–0.3 MΩ). The resulting e-textiles achieve sensing (theoretical limit of detection [LOD] of 0.43 ppm), filtration (adsorption uptake of 1.9 and 0.83 mmol g−1 for MOF powder and MOF/textile, respectively, at 1 bar and 298 K), and detoxification (redox conversion of SO2 gas into solid sulfate) due to the selective material-analyte interactions. This scalable method for generating e-textiles is a promising approach for the fabrication of smart membrane materials with multifunctional performance characteristics.