In this study, CuMt and TiMt montmorillonites were produced via an ion-exchange process with Cu+ and Ti4+ ions. These nanostructured materials were characterized with X-ray diffraction (XRD) and fourier transform infrared spectroscopy (FTIR) measurements and added as nanoreinforcements and active agents in chitosan (CS)/poly-vinyl-alcohol (PVOH)-based packaging films. The developed films were characterized by XRD and FTIR measurements. The antimicrobial, tensile, and oxygen/water-barrier measurements for the evaluation of the packaging performance were carried out to the obtained CS/PVOH/CuMt and CS/PVOH/TiMt films. The results of this study indicated that CS/PVOH/CuMt film is a stronger intercalated nanocomposite structure compared to the CS/PVOH/TiMt film. This fact reflected higher tensile strength and water/oxygen-barrier properties. The antibacterial activity of these films was tested against four food pathogenic bacteria: Escherichia coli, Staphylococcus aureus, Salmonella enterica and Listeria monocytogenes. Results showed that in most cases, the antibacterial activity was generated by the CuMt and TiMt nanostructures. Thus, both CS/PVOH/CuMt and CS/PVOH/TiMt films are nanocomposite candidates with very good perspectives for future applications on food edible active packaging.