Interlayer-polymerization of (3-aminopropyl)trimethoxysilane (APMS) was carried out in the interlayer of lithium hectorite(LHT), and hectorites modified by ''tuning pest'' such as alkylammonium hectorite(CnNHT) and pyridinium hectorite (PyHT). XRD measurements revealed that the polymer-LHT complex showed no d001 diffraction peaks, while the polymer-CnNHT and -PyHT complexes had definite basal spacings depending on the guest or the amount of APMS. The polymer-clay complexes were characterized by means of Si-29 CP/MAS NMR and Fr-IR spectra.