The application of pure chitosan films is significantly limited due to their poor mechanical properties. In this study, a novel type of chitosan/hyperbranched polyethylenimine (CHP) and chitosan/hyperbranched polyethylenimine/Fe3+ (CHPF) films with high toughness and good antibacterial activity were prepared through a noncovalent crosslinking method. From the tensile test results, the strain and toughness of the CHP film increased by 798.1% and 292.3%, respectively, compared with pure chitosan film, after the addition of 20% hyperbranched polyethylenimine (HPEI). The addition of trace metal iron ions (3 mg) forms a metal coordination bond with the amine group on HPEI, as well as the hydroxyl group and amine group on chitosan, and develops a double noncovalent bond network structure with hydrogen bonding, which further enhances the mechanical tensile strength of the chitosan-based film, with an increase of 48.4%. Interestingly, HPEI and Fe3+ can be used as switches to increase and decrease the fluorescence property of chitosan, respectively. Furthermore, the CHP and CHPF films showed good antibacterial activity against S. aureus and E. coli.
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