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Poly(vinylidene fluoride)/organically modified montmorillonites (PVDF/OMMT) nanocomposites with different clay contents were prepared by melt intercalation and compression moulding. The dielectric properties were studied, and the effects of montmorillonites on the crystalline structure of PVDF were characterized, compared and discussed by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy and differential scanning calorimetry (DSC). The results show that the dielectric constant of the PVDF/OMMT nanocomposites is improved. XRD and FTIR results indicate that montmorillonites suppress the formation of α-phase crystals and promote the formation of β-phase crystals. DSC studies suggest that the degree of crystallinity is decreased and the melting and crystallization temperature of nanocomposite are increased compared with those of the pristine PVDF.