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Polymer–silicate nanocomposites were synthesized with atom transfer radical polymerization (ATRP). An ATRP initiator, consisting of a quaternary ammonium salt moiety and an α‐phenyl chloroacetyl chloride moiety, were intercalated into the interlayer spacings of the layered silicate. Subsequent ATRP of styrene with CuCl/2,2′‐bipyridine (bipy) as the catalyst with the initiator‐modified silicate afforded...