Biomineralization-Driven Interfacial Complexation at the Liquid Interface for Probiotic Delivery and Reactive Oxygen Species Scavenging

Integrating functional biomolecules and nanomaterials at liquid interfaces is a fundamental strategy for advancing 3D bioprinting, biocatalysis, and functional interface engineering by synchronizing tunable physical properties of nanomaterials and specialized bioactivities of biomolecules. However, conventional strategies rely on specific surface modifiers that often compromise function and activity of biomolecules and the nanomaterials while impeding interfacial interactions with the surrounding environment. Herein, we introduce a facile, modifier-free approach for constructing biomolecule-nanoparticle integrated functional interfaces by leveraging biomolecule mineralization (preserving native conformation/function) and interfacial complexation with opposing physicochemical properties (facilitating interfacial integration without modifiers). This approach addresses the critical need for modifier-free engineering, ensuring both biomolecular activity and nanoparticle functionality remain fully intact and enabling the interaction between the interface and its surroundings. To demonstrate its utility, we applied this strategy to probiotic delivery: interfacially coanchored mineralized biomolecules and nanozymes, which synergistically enhance probiotic survival and eliminate the reactive oxygen species─which is unattainable with current methods. Therefore, this work establishes a scalable platform for live biotherapeutics, where the intact functionalities of both interfacial biomolecules and nanoparticles are preserved. Beyond therapeutics, the fundamental principle of this strategy can further be extended to applications that require synergistic biomolecule-nanoparticle interactions with high specificity, stability, and scalability, such as advanced biosensing, efficient bioenergy conversion, targeted environmental remediation, and smart biohybrid materials.