The self-driven organization of model protocells intohigher-ordernested cytomimetic systems with coordinated structural and functionalrelationships offers a step toward the autonomic implementation ofartificial multicellularity. Here, we describe an endosymbiotic-likepathway in which proteinosomes are captured within membranized alginate/silkfibroin coacervate vesicles by guest-mediated reconfiguration of thehost protocells. We demonstrate that interchange of coacervate vesicleand droplet morphologies through proteinosome-mediated urease/glucoseoxidase activity produces discrete nested communities capable of integratedcatalytic activity and selective disintegration. The self-drivingcapacity is modulated by an internalized fuel-driven process usingstarch hydrolases sequestered within the host coacervate phase, andstructural stabilization of the integrated protocell populations canbe achieved by on-site enzyme-mediated matrix reinforcement involvingdipeptide supramolecular assembly or tyramine-alginate covalentcross-linking. Our work highlights a semi-autonomous mechanism forconstructing symbiotic cell-like nested communities and provides opportunitiesfor the development of reconfigurable cytomimetic materials with structural,functional, and organizational complexity.
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