The exciting potential of harnessing the synergy between polysaccharides and bioactive components is attracting significant scientific interest. This research paves the way for the development of novel materials that can improve human health. Therefore, current research is conducted to explore the innovative use of chitosan, polyvinyl alcohol (PVA) complex (CHN-PVA), olive oil-stabilized Pickering emulsions (PEs), and films with multifaceted applications. The sonication stabilized Pickering emulsions (PEs at different pH values 3, 5, 7, 9, and 11) exhibited decrease in particle size compared to control PEs. The pH significantly impacted the zeta potential of PEs. Fourier-transform infrared spectroscopy (FTIR) confirmed the non-covalent linkages. The antibacterial activity of the PEs revealed greater efficacy against gram-positive bacteria than gram-negative bacteria. The CHN-PVA synergy greatly impacted the mechanical properties of films, resulting in tremendous increase of tensile strength and elongation at break compared to CHN film. The PEs efficiently delivered quercetin at neutral pH. The electro spraying of PEs significantly extended strawberry shelf life. Finally, the films exhibited promising properties of adsorbent and the results depicted that pH had a significant impact on methylene blue removal. Conclusively, this investigation underscores the potential of CHN-PVA films in food, health, and environmental fields.