Polymeric insulation for HVDC cable is attracting more attention in the modern power transmission system. Especially, the thermoplastic material is desirable for power cable insulation because of its recyclability and ease of processing. Thermoplastic material development is a good alternative to cross-linked polyethylene in the future. Polypropylene has the advantage of avoiding by-products during cable production, which can minimize space accumulation and degassing costs. Therefore, this study investigates the influence of nanofillers on the structural properties of isotactic polypropylene. In addition, the proposed composite material’s morphology, melting, dielectric permittivity, and breakdown strength are examined. Different weight percentages of inorganic nanofillers such as TiO2 and ZnO are used to make nanocomposite thin films. With increasing filler concentration, the dielectric constant of the nanocomposite thin film increases. Apart from that, the dielectric loss of the TiO2 nanocomposite thin film increases with weight percentage initially and it falls nearer to virgin material at a higher frequency. The breakdown strength of the nanocomposite materials shows a similar variation with filler concentration. TiO2 is more resistant to deterioration than ZnO composite. Based on the results of the complete investigation, the TiO2 nanocomposite is better suited for the insulation of HVDC cables.