Polymeric films made from chitosan (CS) doped with metal oxide (MO = cobalt (II) oxide and strontium oxide) nanoparticles at different concentrations (5, 10, 15, and 20% wt. MO/CS) were fabricated with the solution cast method. FTIR, SEM, and XRD spectra were used to study the structural features of those nanocomposite films. The FTIR spectra of chitosan showed the main characteristic peaks that are usually present, but they were shifted considerably by the chemical interaction with metal oxides. FTIR analysis of the hybrid chitosan-CoO nanocomposite exhibited notable peaks at 558 and 681 cm-1. Conversely, the FTIR analysis of the chitosan-SrO composite displayed peaks at 733.23 cm-1, 810.10 cm-1, and 856.39 cm-1, which can be attributed to the bending vibrations of Co-O and Sr-O bonds, respectively. In addition, the SEM graphs showed a noticeable morphological change on the surface of chitosan, which may be due to surface adsorption with metal oxide nanoparticles. The XRD pattern also revealed a clear change in the crystallinity of chitosan when it is in contact with metal oxide nanoparticles. The presence of characteristic signals for cobalt (Co) and strontium (Sr) are clearly shown in the EDX examinations, providing convincing evidence for their incorporation into the chitosan matrix. Moreover, the stability of the nanoparticle-chitosan coordinated bonding was verified from the accurate and broadly parametrized semi-empirical tight-binding quantum chemistry calculation. This leads to the determination of the structures' chemical hardness as estimated from the frontier's orbital calculations. We characterized the dielectric properties in terms of the real and imaginary dielectric permittivity as a function of frequency. Dielectric findings reveal the existence of extensive interactions of CoO and SrO, more pronounced for SrO, with the functional groups of CS through coordination bonding. This induces the charge transfer of the complexes between CoO and SrO and the CS chains and a decrease in the amount of the crystalline phase, as verified from the XRD patterns.