TPS/CTS based materials were prepared using a twin-screw extruder and then converted into a film by blown film extrusion. FTIR results showed that chitosan could form hydrogen bond interaction with starch, resulting in decreased V-type crystallinity and positive effects on film properties. The addition of 0.37–1.45% of chitosan improved strength (tensile strength increased ∼8–97%), stiffness (Young's modulus increased ∼40–154%), and thermal stability as well as reduced water absorption of the TPS film. However, extensibility of TPS film decreased (elongation at break decreased ∼5–73%) when chitosan was incorporated. Compared with TPS film, TPS/CTS films were a more intense yellow with increased opacity, and also showed greater UV absorption.