Interlayer surfaces of layered double hydroxide (LDH) have been functionalized with amine moieties by condensation between the hydroxyl groups and (3-aminopropyl)triethoxysilane (APS) molecules via the covalent oxane bonds M-O-Si (M=Zn and Cr) (see Figure). Since the galleries of the modified LDHs have a hydrophobic field, various functional molecules such as enzymes, catalysts, and organic molecules can be incorporated between the LDH layers.