Low cost and scalable manufacturing of highly doped cellulose for enhanced multifunctional applications is still an issue. In this work, eco-friendly nanocomposites were fabricated by incorporating regenerated cellulose (RC) of 10, 30, and 50 wt% into an exfoliated graphene nanoplatelets (GNPs), resulting in the intercalation of GnPs. The thermal and electrical properties of hybrid nanocomposites were investigated. The structural property was conducted through scanning electron microscope and X-ray diffraction analyses. Strong frequency-dependent dielectric response was found due to the change of the permittivity and the loss tangent of nanocomposites by different content of RC, which is associated with the polarizations behavior. Non-elastic relaxation at the GNPs–RC chains interfacial areas in an alternating field was identified as the main cause of polarization losses among others. Detailed ferroelectric measurements provided the evidence of the ideal resistive behavior of the nanocomposites, which are confirmed by the resistivity measurements along the out-of-plane direction of the nanocomposite sheets.