The aim of the study is to determine the effect of the vermiculite (Vk) and its organoclays, which were prepared by using cationic and anionic surfactants, on polyvinylbutyral (PVB) nanocomposites. The PVB nanocomposites were synthesized by using solution casting method, concerning the changes on the mechanical, and thermal properties of PVB. Modification of vermiculites with surfactant extends the interlayer space of the vermiculite and increases the interactions of vermiculite and PVB. The structural, morphological characterizations of PVB nanocomposites were examined by XRD (X-ray diffraction), and TEM (Transmission electron microscopy), and mechanical, thermal properties of the nanocomposites were determined by DMA (Dynamical mechanical analysis), and DSC (Differential scanning calorimetry) methods. The results showed that addition of vermiculite or modified vermiculite increased the elastic modulus of PVB. Modification of vermiculite with anionic surfactant resulted in a better exfoliation and improved the mechanical and thermal properties compared with modification of vermiculite with cationic surfactant in PVB nanocomposites.