A novel reactive layered two-dimensional molecular space material [layered chloroacetamide phenyl silica (CAAPhS)] with regular chlorine groups was synthesized by grafting chlorine groups into the layer structure of layered aminophenyl silica. The reactive activity of chlorine groups regularly arranged in the layer structure of layered CAAPhS was confirmed through a substitution reaction with n-butylamine. Layered CAAPhS showed potential as a starting material for the formation of a series of two-dimensional layered materials with various regular functional molecules and organic-inorganic composite materials. (C) 2007 Elsevier Inc. All rights reserved.