Electrospun chitosan (Cs) fibers were deposited with titanium dioxide particles through plasma- enhanced chemical vapor process using a compact planar magnetron device. Molecular constructs of Cs and Cs-TiO were modeled using the Gaussian software package to investigate their physicochemical properties and establish the mechanism of interaction between biopolymer and metal oxide. XRD crystalline peak at confirmed the integration of into the chitosan fibers. Both experiment and simulation confirmed Cs and combined to become one composite unit Cs-TiO via the glycosidic bond C-O-C of the glucose ring. FTIR and simulated vibrational spectra showed band splittings at 978 and , respectively, which suggests the integration and intermolecular attraction between Cs and at said linkage. SEM shows beads of 100-200 nm sizes scattered over the chitosan fibers. The molecular model of Cs-TiO showed optimized geometry with larger dipole moment, higher negative energy, lower ionization potential and narrower HOMO-LUMO energy gap compared to pure Cs; indicative of a resultant composite with enhanced structure and reactivity. Composites synthesized at longer plasma treatment time showed better dispersion of deposits exhibiting higher antimicrobial power with inhibition zones approximately 11.5 mm in diameter.