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Characterization of broadband dielectric behaviour of polymer nanocomposites (PNCs) is vital for the exploration of efficient nanodielectrics as energy storage, flexible dielectric substrates, and insulators in a wide range of advanced electronic device technologies. Accordingly, herein, PNC films based on poly(vinylidene fluoride) (PVDF) and poly(methyl methacrylate) (PMMA) blend matrix (80/20 wt/wt%) dispersed with 0, 2.5, 5, and 10 wt% organo-modified montmorillonite (OMMT) nanoclay are developed by state-of-the-art homogenized solution casting method. These PVDF/PMMA/OMMT compositions based flexible PNC films are characterized in detail by employing a scanning electron microscope (SEM) equipped with energy dispersive X-ray (EDX) device, X-ray diffractometer (XRD), Fourier transform infrared (FTIR) spectrometer, differential scanning calorimeter (DSC), inductance-capacitance-resistance (LCR) meter, and impedance/material analyzer (IMA). The SEM microimages, XRD traces, and FTIR spectra evidenced appreciable homogeneity and surface morphology, intercalated and exfoliated OMMT structures, and the α, β, and γ-phase crystallites of the PVDF in these complex semicrystalline PNCs. The DSC thermograms confirmed a significant alteration in the melting temperature and degree of crystallinity of the PVDF crystallites with the increased amount of OMMT in the 80PVDF/20PMMA blend host matrix. The broadband dielectric dispersion spectra over the frequency range of 20 Hz - 1 GHz explained the contribution of interfacial polarization in the complex dielectric permittivity at lower experimental frequencies, whereas at higher frequencies permittivity is ruled by dipolar polarization in these composites at 27 oC. The dielectric loss angle tangent and electric modulus spectra revealed an intense structural dynamics relaxation process in the radio frequency region. The influence of OMMT concentration on the dielectric permittivity and electrical conductivity is explored. The detailed dielectric and electrical characterization of these innovative semicrystalline composites with important structural and thermal properties revealed their immense potential as high-performance nanodielectrics for highlighting current applications of broadband frequency range electrical and electronic device technologies.