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While metal-organic frameworks (MOFs) show great potential for gas adsorption and storage, their powder form limits deployment opportunities. Integration of MOFs on polymeric fibrous scaffolds will enable new applications in gas adsorption, membrane separation, catalysis, and toxic gas sensing. Here, we demonstrate a new synthesis route for growing MOFs on fibrous materials that achieves high MOF loadings, large surface areas and high adsorptive capacities. We find that a nanoscale coating of Al2O3 formed by atomic layer deposition (ALD) on the surface of nonwoven fiber mats facilitates nucleation of MOFs on the fibers throughout the mat. Functionality of MOFs is fully maintained after integration, and MOF crystals are well attached to the fibers. Breakthrough tests for HKUST-1 MOFs [Cu3(BTC)2] on ALD-coated polypropylene fibers reveal NH3 dynamic loadings up to 5.93 ± 0.20 mol/kg(MOF+fiber). Most importantly, this synthetic approach is generally applicable to a wide range of polymer fibers (e.g., PP, PET, cotton) and MOFs (e.g., HKUST-1, MOF-74, and UiO-66).