Our study investigates the interaction between tannic acid (TA) and chitin nanofibers (ChNF) through surface/interfacial tension, rheology, electrokinetic analyses, quartz crystal microgravimetry, and molecular dynamics simulations. We propose a method using edible phenolic acids as interfacial modifiers to enhance nanochitin adsorption at oil-water interfaces, focusing on high internal phase Pickering emulsions (HIPPE). Our results emphasize charge neutralization and reduced interfacial tension as crucial for the high stability of ChNF-TA co-assemblies. TA demonstrates rapid and extensive adsorption onto ChNF, achieving adsorption amounts up to 450 ng/cm2. HIPPEs stabilized with ChNF-TA complexes exhibit outstanding performance in food-safe extrusion, producing self-supporting materials with high fidelity. These emulsions maintain dimensional stability after two months of storage and readily transform into cryogels via freeze-drying. Leveraging their stability and viscoelastic properties, HIPPEs stabilized with ChNF-TA offer significant potential for developing green emulsions, which can be further tailored for personalized nutrition design.
