The purpose of the present research is to obtain waste of polymeric composite as an insulator capacitive application. Rubber materials, once they end their useful life, may be difficult to reuse or recycle. At present, research only uses one tire recycling method, which involves grinding and separating steel and fibers from vulcanized rubber, and then using the rubber particles for industrial capacitors. The methodology for this research is to compare the permittivity (ε′ and ε″) between high-density polyethylene (HDPE) and the polymer matrix compound, consisting of an HDPE polymeric matrix blended with end-of-life tire particles (ground tire rubber (GTR)), to analyze the feasibility of using such tires as electrically insulating materials (dielectrics). The incorporation of carbon black in the GTR compounds modifies conductivity; GTRs carry a significant amount of carbon black, and therefore some electrical properties may change significantly compared to highly insulating polymer substrates. The performed experimental study is based on a dynamic electric analysis (DEA) test developed in the frequency range of 10−2 Hz to 3 MHz and at different temperatures (from 35 to 70 °C) of different samples type: HDPE neat and HDPE compounds with 10%, 20% and 40% of GTR loads. A sample’s electrical behavior is checked for its dependence on frequency and temperature, focused on the permittivity property; this is a key property for capacitive insulators and is key for examining the possible applications in this field, for HDPE + GTR blends. Results for the permittivity behavior and the loss factor show different electrical behavior. For a neat HDPE sample, no dependence with frequency nor temperature is shown. However, with the addition of 10%, 20%, and 40% amount of GTR the HDPE compounds show different behaviors: for low frequencies, interfacial polarization relaxation is seen, due to the Maxwell–Wagner–Sillars (MWS) effect, performed in heterogeneous materials. In order to analyze thermal and morphological properties the differential scanning calorimetry (DSC) test and scanning electron microscopy (SEM) have been used. Results obtained show that adding waste tire particles in an HDPE matrix allows HDPE + 40% GTR blends to act as a dielectric in capacitors, increasing the capacitor dielectric efficiency in the low frequencies due to the MWS effect, which increases the dielectric constant.