Architected Living Materials with Embedded Microdroplets Hosting Microbial Consortia for Continuous Flow Biocatalysis

Abstract Living materials that integrate microbial consortia within synthetic scaffolds offer powerful capabilities for biocatalysis, but preserving biological activity alongside spatial structure remains a major challenge. Here, we present a strategy that embeds phase‐separated aqueous microdroplets within a 3D‐printable hydrogel matrix to create architected living materials. Aqueous two‐phase immiscibility between the droplet core and scaffold‐forming polymers ensures physical separation, maintaining discrete liquid microenvironments essential for microbial viability and metabolic cooperation. The resulting materials exhibit excellent structural fidelity, cell retention, and mechanical resilience while enabling programmable microbial organization. When implemented under continuous flow conditions, the material supports long‐term biocatalysis of a mutualistic pairing of Chlorella vulgaris and Bacillus subtilis and the degradation of azo dyes in synthetic wastewater. This strategy introduces a generalizable route for constructing compartmentalized living materials, enabling the structured deployment of microbial consortia for chemical biotransformation and process‐scale applications.