Polymers have gained attraction at the industrial level owing to their elastic and lightweight nature, as well as their astonishing mechanical and electrical applications. Their scope is limited due to their organic nature, which eventually leads to the degradation of their properties. The aim of this work was to produce polymer composites with finely dispersed metal oxide nanofillers and carbon nanotubes (CNTs) for the investigation of their charge-storage applications. This work reports the preparation of different polymeric composites with varying concentrations of metal oxide (MO) nanofillers and single-walled carbon nanotubes (SWCNTs). The successful synthesis of nanofillers (i.e., NiO and CuO) was carried out via the sonication and precipitation methods, respectively. After, the smooth and uniform polymeric composite thin films were prepared via the solution-casting methodology. Spectroscopy and diffraction techniques were used for the preliminary characterization. Scanning electron microscopy was used to check the dispersion of carbon nanotubes (CNTs) and MOs in the polymer matrix. The addition of nanofillers and carbon nanotubes (CNTs) tuned the bandgap, reduced the strain, and enhanced the elastic limit of the polymer. The addition of CNT enhanced the mechanical strength of the composite; however, it increased the conductivity, which was tuned by using metal oxides. By increasing the concentration of NiO and CuO from 2% to 6% bandgap of PVA, which is 5–6 eV reduced to 4.41 and 4.34 eV, Young’s moduli of up to 59 and 57.7 MPa, respectively, were achieved. Moreover, improved dielectric properties were achieved, which shows that the addition of metal oxide enhances the dielectric behavior of the material.

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