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This study investigates the effect of clay addition on the broadband dielectric properties of multi-walled carbon nanotube/polyvinylidene fluoride (MWCNT/PVDF) composites, that is, frequency range of 101−106 Hz. Different loadings of MWCNT and clay were used for the preparation of three-phase (MWCNT/Clay/PVDF) nanocomposites via melt-mixing method. The crystalline structure and morphology of nanocomposites were examined by employing characterization techniques such as X-Ray diffraction, transmission electron microscopy, and differential scanning calorimetry. The dielectric spectroscopy showed that introducing clay into the MWCNT/PVDF nanocomposites at a critical MWCNT concentration improved dielectric properties tremendously. It was interestingly observed that the incorporation of a specific amount of clay, that is, 1.0 wt%, into the (MWCNT/PVDF) nanocomposite at a critical MWCNT loading, that is, 0.5 wt% MWCNT, resulted in a huge increase in the dielectric permittivity (670% at 100 Hz) and a considerable reduction in the dissipation factor (68% at 100 Hz). POLYM. COMPOS., 2014. © 2014 Society of Plastics Engineers