A novel two-dimensional molecular space (layered carboxylpropylamidephenylsilica, CPAPhS) with regular carboxyl groups was successfully synthesized through grafting carboxyl groups in the structure of layered (aminophenyl)silica using butanedioic anhydride. The carboxyl groups regularly arranged in the layered CPAPhS can react with various organic molecules with amino and hydroxyl groups through formation of reactive intermediate with catalyzers, such as SOCl2. In this research, an example was used to prove the reaction properties of regular carboxyl groups in layered CPAPhS. The layered CPAPhS was reacted with SOCl2 to form layered acyl chloridepropylamidephenylsilica (ACPAPhS) and then reacted with n-butylamine and n-butyl alcohol to form layered n-butylamidepropylamidephenylsilica (BAPAPhS) and n-butylesterpropylamidephenylsilica (BEPAPhS) with regular molecular structures. Layered CPAPhS showed the potential as a starting material for formation of a series of novel two-dimensional molecular space with various regular molecular structures, and as a solid acceptor for chemical reagent with amino and hydroxyl groups for chemical processes.