A peelable gel coating based on a curable ammonium-alcohol ionic liquid (IL) prepolymer has been developed for the decontamination of toxic industrial chemicals (TICs) from porous substrates. The physical properties of these coatings can be tuned by controlling the prepolymer molecular weight (prepared by RAFT polymerization) and by altering the formulation of the initial coating mixture. The initially applied (uncured) solutions can be applied onto porous wood and ceramic substrates with minimal soak-in, and these films cure quickly in situ under ambient conditions. These coatings were tested in a series of assays meant to demonstrate their effectiveness as TIC vapor barriers and materials that absorb liquid TICs from the aforementioned substrates. The coatings were found to suppress similar to 80% of the vapor released by a TIC simulant (o-dichlorobenzene) from these substrates and to extract up to 85% of the mass of the originally applied simulant that soaked into these substrates.