Emergent Motility of Self‐Organized Particle‐Giant Unilamellar Vesicle Assembly

Giant unilamellar vesicles (GUVs), soft cell-sized compartments formed through the self-assembly of lipid molecules, have long been utilized as model systems and passive carriers in membrane biophysics and biomedical applications. However, their potential as dynamically responsive and motile systems remains largely untapped due to challenges in achieving controlled and sustained motion in soft, deformable structures. Here, an autonomous cell-like microrobot through the emergent self-assembly of GUVs (5-10 µm) and silica microparticles (1-3 µm) under alternating current electric fields is realized. Self-propulsion arises from asymmetric self-organization of the particles on the vesicle surface, enabling a reversible transformation of the assembly into an active structure. Unlike rigid colloidal systems, GUVs introduce unique features enabled by their soft lipid membranes: shape deformations, membrane tension-dependent motility, and field-triggered live bacteria release via vesicle bursting. Through experiments and simulations, the mechanisms underlying self-assembly and propulsion are investigated, and a dynamic phase diagram is constructed to map the motion regime as a function of field parameters. Finally, it is shown that these self-assembled structures are capable of reconfiguration in response to local constraints in the environment, suggesting potential applications in complex environments and advancing the potential of GUVs toward the rational design of cell-like microrobots or artificial cell systems.