In this study, we incorporated 2,3-dialdehyde nanocrystalline cellulose (DANC) into chitosan as a reinforcing agent and manufactured biodegradable films with enhanced gas barrier properties. DANC generated via periodate oxidation of cellulose nanocrystal (CNC) was blended at various concentrations with chitosan, and bionanocomposite films were prepared via casting and characterized systematically. The results showed that DANC developed Schiff based bond with chitosan that improved its

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... significantly. The addition of DANC dramatically improved the gas barrier performance of the composite film, with water vapor permeability (WVP) value decreasing from 62.94 g·mm·m−2·atm−1·day−1 to 27.97 g·mm·m−2·atm−1·day−1 and oxygen permeability (OP) value decreasing from 0.14 cm3·mm·m−2·day−1·atm−1 to 0.026 cm3·mm·m−2·day−1·atm−1. Meanwhile, the maximum decomposition temperature (Tdmax) of the film increased from 286 °C to 354 °C, and the tensile strength of the film was increased from 23.60 MPa to 41.12 MPa when incorporating 25 wt.% of DANC. In addition, the chitosan/DANC (75/25, wt/wt) films exhibited superior thermal stability, gas barrier, and mechanical strength compared to the chitosan/CNC (75/25, wt/wt) film. These results confirm that the DANC and chitosan induced films with improved gas barrier, mechanical, and thermal properties for possible use in film packaging.