Synergistic Bioinspired Interface and Segregated Graphene Oxide Networks Enabling Enhanced Mechanical Strength and Chemical Resistance in Natural Rubber Latex Composites

Natural rubber (NR) latex is a renewable colloidal dispersion used in medical gloves, coatings, and flexible products. It is known for its excellent elasticity and film-forming ability but is limited by insufficient mechanical robustness and chemical resistance. Incorporating nanofillers, such as graphene oxide (GO), is an effective approach to enhance its performance; however, achieving strong interfacial compatibility between hydrophilic GO and the nonpolar rubber matrix remains challenging. To overcome this issue, a multifunctional interfacial design inspired by mussel adhesion chemistry was developed to construct a hierarchical and cohesive GO network within the NR latex matrix. A tannic acid-based modifier (TM) bearing catechol and thiol groups was synthesized and anchored onto latex particles via hydrogen bonding with surface proteins and phospholipids, enabling subsequent π – π interactions and hydrogen bonding with GO nanosheets. This guided the selective self-assembly of GO into a continuous segregated network along the latex particle boundaries. Hierarchical interface reinforcement was achieved through Eu 3+ ligand coordination. The incorporation of GO and enhancement of interfacial interactions promoted strain-induced crystallization, resulting in increased crystallinity and improved load transfer. The resulting composite film containing 0.5 part per hundred rubber GO and the bioinspired interface exhibited a tensile strength that was 107.8% higher than that of the pure NR latex film, while maintaining an elongation at break of 915%. Tear strength increased by 118.5%, toughness reached 61.7 MJ/m 3 , nitrogen permeability decreased by 20.1%, and antibacterial efficiency against both Escherichia coli and Staphylococcus aureus reached 99.9%. The films also exhibited enhanced resistance to organic solvents, acids, and alkalis. This study provides a green and scalable strategy for fabricating high-performance NR latex-based products suitable for medical, protective, and engineering applications.