The direct interlamellar silylation of synthetic gyrolite with n-butyldimethylchlorosilane was carried out. The silylation reaction was performed in two stages at temperatures of 50 degrees C and 60 degrees C, respectively. In the first stage of the reaction process, silylation was confined predominantly to the interlayer sheet, resulting in the formation of 3:2 organo-phyllosilicates. In the second stage of the reaction, the silylation depleted the brucite-like calcium oxide (hydroxide) sheets within the 3:2 organo-phyllosilicates, leading to the formation of organic polysiloxane sheets characterized by a modification of the original silicate structure. The synthesized gyrolite and silylated derivates formed in the two-stage reaction process were characterized using XRD, (29)Si MAS NMR, FTIR, SEM, and elemental analysis techniques. (C) 2011 Elsevier B.V. All rights reserved.