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Although the performance of smart textiles would be enhanced if they could display self-cleaning ability toward various kinds of contamination, the procedures that have been used previously to impart the self-cleaning potential to these functional fabrics (solvent casting, dip coating, spin coating, surface crosslinking) have typically been expensive and/or limited by uncontrollable polymer thicknesses and morphologies. In this paper, we demonstrate the use of atomic transfer radical polymerization for the surface-initiated grafting of po