Bioplastic has been perceived as a promising candidate to replace petroleum-based plastics due to its environment-friendly and biodegradable characteristics. This study presents the chitosan reinforced starch-based bioplastic film prepared by the solution casting and evaporation method. The effects of processing parameters, i.e., starch concentration, glycerol loading, process temperature and chitosan loading on mechanical properties were examined. Optimum tensile strength of 5.19 MPa and elongation at break of 44.6% were obtained under the combined reaction conditions of 5 wt.% starch concentration, 40 wt.% glycerol loading, 20 wt.% chitosan loading and at a process temperature of 70 °C. From the artificial neural network (ANN) modeling, the coefficient of determination (R²) for tensile strength and elongation at break were found to be 0.9955 and 0.9859, respectively, which proved the model had good fit with the experimental data. Interaction and miscibility between starch and chitosan were proven through the peaks shifting to a lower wavenumber in FTIR and a reduction of crystallinity in XRD. TGA results suggested the chitosan-reinforced starch-based bioplastic possessed reasonable thermal stability under 290 °C. Enhancement in water resistance of chitosan-incorporated starch-based bioplastic film was evidenced with a water uptake of 251% as compared to a 302% registered by the pure starch-based bioplastic film. In addition, the fact that the chitosan-reinforced starch-based bioplastic film degraded to 52.1% of its initial weight after 28 days suggests it is a more sustainable alternative than the petroleum-based plastics.