Poly(ethylene oxide) (PEO)/organomodified-montmorillonite (OMMT) nanoclay based nanocomposites having 1, 3, 5, 10, and 20 wt% OMMT nanofiller were prepared by homogeneous mixing and the melt-compounding method. These hybrid materials were characterized by employing X-ray diffractometer, differential scanning calorimeter, and radio frequency impedance analyzer. The experimental results confirmed the formation of OMMT intercalated structures with reduced crystallinity and increased melting temperature of PEO crystallites which are predominantly ruled by the nanofiller amounts in the PEO/OMMT nanocomposites. Dielectric permittivity of these nanocomposites measured at 20 C exhibited a gradual decrease with increasing frequencies of the applied harmonic electric field of high to ultrahigh range (i.e., 1 MHz-1 GHz), but it changed anomalously in the range of 2.6-3.6 with the increase of OMMT amounts in the PEO matrix. The dielectric losses in these composites were found low and their loss spectra exhibited a hydrogen bond dipolar reorientation relaxation process around 1 GHz. The alternating current electrical conductivity of these nanocomposites increased with frequency and also changed with the OMMT concentrations. These PEO/OMMT nanocomposites are classified as low permittivity nanodielectrics which could be potential candidates for advances in flexible and biodegradable radio-electronic devices.