The extensive use of nondegradable plastic tableware has brought serious environmental problems. Starch-based materials are good alternatives to plastics, but poor mechanical properties and intrinsic hydrophilicity limit their utilizations. In order to address this issue, naturally abundant bagasse pulp fiber is used as the reinforcing agent to improve the mechanical properties of starch and polydimethylsiloxane coating (CSB 35 -PDMS 50 ) to improve their hydrophobicity and hydrostability. CSB 35 -PDMS 50 reaches the tensile strength of 21.2 MPa and contact angle of 121°. The enhancement of the mechanical strength can be explained by strong hydrogen bonding between starch and cellulose, as indicated by noncovalent interaction-reduced density gradient (NCI-RDG) analysis. CSB 35 -PDMS 50 retains the low water adsorption rate within 60 h, remains stable in water for 24 h without morphology change, and maintains initial hydrophobicity after continuous abrasion in sandpaper and high-pressure water spraying due to the formation of Si─O-C bonds. The water absorption capacity of CSB 35 -PDMS 50 is less than 10% when used as the cap materials for Eppendorf tube for 30 days. Furthermore, CSB 35 -PDMS 50 demonstrates good biodegradability in the soil with 74% in 100 days. The tableware prepared from ther composites demonstrates good potentials as the competitive substitute for plastics with easy production, high strength, and biodegradability.

Starch‐based materials have been proposed as the alternatives to plastic tableware and packaging materials; however, starch materials suffer from poor wear resistance because of their hydrophilicity. Therefore, it is essential to prepare starch composites with hydrophobic functionalization especially using fluorine‐free compounds. In this study, superhydrophobic starch–cellulose composites are fabricated by using polyethyleneimine (PEI) as the adhesive layer and beeswax as the functionalized layer. The superhydrophobicity (contact angle: 152°) is achieved by building the rough surface and low surface energy of beeswax. Meanwhile, polyethyleneimine tightly connects the beeswax coating and the starch composites by hydrogen bonding, and the surface remains superhydrophobic even after 200 s of water impact. The water/moisture absorption reduced significantly (>30%) after beeswax functionalization thanks to the increased hydrophobicity while the mechanical strength keeps the same (≈22 MPa) compared with the unfunctionalized sample. The self‐cleaning study on various types of liquid drinks (milk, cola, coffee, tea) on the superhydrohobic starch composites demonstrates efficient repellence to the fluids and retains the superhydrophobicity upon different liquid. The durable and biodegradable starch–cellulose composites with excellent self‐cleaning and antifouling performance provide the methodological basis for developing next‐generation green packaging materials over common plastics.

The production of paper‐based food packaging materials is of vital importance as the release of microplastics into aqueous environment and food chain has aroused significant public concern. In this study, antibacterial pulp board was demonstrated by co‐spraying chitosan (CS) and ε‐polylysine (ε‐PL) on wet sheet and dried to form fibrous pulp board (ε‐PL‐CS). ε‐PL functionalization showed great antibacterial performance while its hydrophilicity limited its further application for food packaging. Interestingly, ε‐PL‐CS pulp board not only demonstrated excellent antibacterial performance (99.99% against both bacteria Staphylococcus aureus and Escherichia coli), but also maintained high hydrophobicity (ca. 135°) and water resistance due to the positive charge of ε‐PL and CS as well as penetration of CS into pulp board. In addition, CS functionalization significantly improved the mechanical strength of the pulp board by around 100% (20 MPa). More importantly, the ε‐PL‐CS pulp board could successfully prevent bacteria growth within 15 days at room temperature due to their high hydrophobicity and smooth surface, indicating the long‐term stability as packaging materials. Satisfactory strawberry storage stability of ε‐PL‐CS cardboard lunch box provided great application promise for the development of antimicrobial packaging materials.