Emulsion interfacial nanoarchitectonics with a biomimetic channel‐architected polymer for enhanced biocatalysis

Overcoming mass transfer limitations at the water–organic interface is critical in biphasic biocatalysis. Inspired by the natural cellular processes such as endocytosis and transport proteins, we developed an amphiphilic polymer with jellyfish‐like nanoarchitectonics to engineer the emulsion interface. This polymer forms dynamic micelles to compartmentalize hydrophobic compounds and creates channel‐like structures that facilitate substrate transfer across the phase boundary. Compared to the single‐chain polymer, the jellyfish‐inspired emulsifier significantly enhanced the biphasic biotransformation across diverse reactions. In the un‐emulsified systems, the channel‐structured polymer boosted the yield of the benzaldehyde lyase‐catalyzed benzoin condensation reaction by over 50% relative to controls. In the emulsified systems, a 77% higher efficiency was achieved in the multi‐enzyme cascade reaction involving aromatic and aliphatic substrates, underscoring its versatility. This work bridges the gap between polymer architecture design and biocatalytic performance, offering a biomimetic strategy to engineer emulsion interfaces for revolutionizing mass transfer in biphasic systems.