<p>Polymer nanocomposites are proposed as potential candidates for energy storage devices. The present work includes enhancing the piezoelectric response of chitosan-ZnO (CS-ZnO) thin films and chitosan-TiO₂-coated ZnO (CS-TZO) nanocomposite films. ZnO and TZO-incorporated chitosan polymer nanocomposite thin films were successfully synthesized and investigated for structural, dielectric, ferroelectric, and piezoelectric response. The effect of unifying ZnO and TZO nanoparticles (NPs) as chitosan nanofillers is covered in this study. By experimentation, pristine and surface-decorated chitosan thin films were synthesized. Structural studies were carried out with X-ray diffraction analysis. The surface morphology of chitosan thin films was examined through a Field emission scanning electron microscope. The outcomes of this work demonstrated that CS-TZO advanced polymer nanocomposites are promising candidates for enhanced energy storage devices. The energy storage density calculations were carried out which revealed that pristine CS displayed <i>U</i>_D = 31.2&#xa0;μJ/cm³, whereas CS-ZnO thin film demonstrated <i>U</i>_D = 50.8&#xa0;μJ/cm³. The evaluated value of energy storage density (<i>U</i>_D) for CS-TZO composite film was found to be 59.9&#xa0;μJ/cm³. The improved performance of CS-TZO composite film is attributed to which thereby confirming the effect of TiO₂ coating on ZnO nanoparticles, which induces interfacial polarization and facilitates efficient charge storage. The enhanced energy density of CS-TZO composite film depicts promising candidature for advanced and eco-friendly energy storage applications.</p>