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.