The purpose of this research work was to synthesis bioderived nanocomposite films by incorporating Na_0.5Bi_0.5TiO₃ (NBTO) nanoparticles into a chitosan matrix. The NBTO nanoparticles were synthesized using a traditional solid-state technique. Then, through a solution-casting approach, flexible composite films were fabricated using chitosan polymer. The study presents a range of compelling findings. For structural and morphological insights, scanning electron microscopy (SEM) reveals a fascinating morphology where NBTO nanoparticles are uniformly dispersed and interlocked with other particles, forming interconnected grains with significant interspaces within the chitosan matrix. For the optical properties, the spectral response within the 300–800 nm range is primarily governed by light scattering attributed to NBTO particles with diameter sizes ranging from 100 to 400 nm, as well as the distinctive bandgap exhibited by the NBTO phase. The investigation of dielectric properties demonstrates that composite films exhibit markedly higher dielectric values in comparison to pure chitosan films. It is noteworthy that an increase in the NBTO content results in a corresponding increase in dielectric values, enhancing the versatility of these materials. Local piezoelectric measurements utilizing piezoresponse force microscopy confirm the expected piezoelectric and ferroelectric behavior of NBTO particles when dispersed within the chitosan matrix. This research introduces a novel class of biocompatible nanocomposite materials, combining impressive structural attributes, enhanced dielectric properties, and piezoelectric capabilities. The outcomes of this study hold substantial promise for advanced applications in opto- and piezoelectric technologies, marking a significant advancement in biologically sourced materials with multifunctional properties.