Dynamic Co‐Clustering and Self‐Sorting in Interactive Protocell Populations

The design and implementation of collective actions in model protocell communities is an on-going challenge in synthetic protobiology. Herein, we covalently graft alginate or chitosan onto the outer surface of semipermeable enzyme-containing silica colloidosomes to produce hairy catalytic protocells with pH-switchable membrane surface charge. Binary populations of the enzymatically active protocells exhibit self-initiated stimulus-responsive changes in spatial organization such that the mixed community undergoes alternative modes of electrostatically induced self-sorting and reversible co-clustering. We demonstrate that co-clustering, but not self-sorting, mitigates signal attenuation in a binary community of enzyme-containing sender and receiver protocells due to increased proximity effects. The level of signal attenuation is correlated with a time-dependent pH-mediated switch in the spatial organization of the sender and receiver populations. Our results pave the way towards the development of programmable networks of adaptive life-like objects and could have implications for the development of interactive cytomimetic materials and agent-based robotics.