Interfacial assembly of biomimetic MOF-based porous membranes on coacervates to build complex protocells and prototissues.

The bottom-up construction of cell-like entities or protocells is essential for emulating cytomimetic behaviours within artificial cell consortia. Complex coacervate microdroplets are promising candidates for primordial cells; however, replicating the complex cellular organization and cell-cell interactions using membraneless coacervates remains a major challenge. To address this, we developed membrane-bound coacervate protocells by interfacial assembly of metal-organic framework nanoparticles around coacervate microdroplets. By leveraging the inherently porous structure and surface chemistry of metal-organic frameworks, we demonstrated the ability to regulate biomolecular organization within the protocells and integrate proteins into the membrane, thereby imitating both integral and peripheral membrane proteins. These membranized coacervates were further engineered into artificial-organelle-incorporated protocells and tissue-like assemblies capable of signal processing and protocell-to-protocell communication. Our findings highlight the potential of designing artificial systems with spatially controlled biomolecular organization to mimic natural cellular functions, paving the way for the assembly of membranized coacervates into prototissues.