Shirui Li, Xinyue Tang, Wenyu Hui, Yiran Tan, Zixi Gao, Jiachang Feng, He Wang
The development of biodegradable active packaging that combines mechanical robustness with sustained antimicrobial functionality remains challenging. This study reports a multifunctional active film integrating a polylactic acid/bacterial cellulose (PLA/BC) composite substrate with surface-confined bioactivity via layer-by-layer (LbL) assembly. Citral-loaded whey protein concentrate and chitosan were sequentially deposited to spatially decouple structural reinforcement from antimicrobial function. The optimized multilayer film exhibited a compact stratified architecture with strong interlayer adhesion, high tensile strength (42.14 MPa), enhanced oxygen barrier performance (peroxide value, 9.11 meq/kg), and pronounced antifungal activity against Penicillium expansum and Aspergillus niger. Moreover, the LbL coating enabled sustained and simulant-responsive citral release, alleviating rapid volatilization associated with bulk incorporation. Bread storage tests demonstrated delayed mold development and improved textural and microstructural stability, resulting in an extended mold-free shelf life relative to uncoated PLA/BC films and commercial polyethylene packaging. Overall, this hierarchical design provides a viable strategy for sustainable active food packaging.