| Summary: | ZnO-doped Polyvinyl alcohol/polyvinyl pyrrolidone (PVA/PVP) polymeric films were prepared in this study through an easy and inexpensive solution-casting method. The scope of the study was based on the structural, dielectric, and optical parameters, as well as on the optical limiting effects of the ZnO-doped polymer blend (PB) as nanocomposite films. The X-ray diffraction (XRD) analysis indicated that the synthesized nanocomposites were semicrystalline. The calculated crystalline size of the polymeric semicrystalline peak decreased as ZnO increased or enhanced the blend polymer. Fourier’s transformer infrared (FT-IR) study confirmed a substantial dispersion of ZnO nanoparticles in a polymeric PVA/PVP matrix. The optical absorption properties suggested focusing on the surface plasmonic peak (SPR). The refractive index values ranged from 1.718 for the pure PB ZnO<sub>0</sub> sample in the Hossam, Ibrahim, and Heba model to 3.036 for the PB ZnO<sub>5</sub> film from the Anani model. Nonlinear optical parameters (<inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi mathvariant="sans-serif">χ</mi></semantics></math></inline-formula>((3)), and n(2)) were calculated and analyzed for the PB ZnO nanocomposite films under investigation. The maximum value for <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi mathvariant="sans-serif">χ</mi></semantics></math></inline-formula>((1)) was 0.550, while for <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mi mathvariant="sans-serif">χ</mi></semantics></math></inline-formula>((3)), its susceptibility value was 155.85 × 10<sup>−13</sup> esu, and for the nonlinear refractive index (n((2)), it was 20.87 × 10<sup>−11</sup> esu. A gradual decrease was revealed in the optical limiting sources, as a high content of ZnO was induced in the blend PVA/PVP polymer. Due to their unique properties, these materials can be used in electronic and optoelectronic devices.
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