Producing artificial multicellular structures to process multistep cascade reactions and mimic the fundamental aspects of living systems is an outstanding challenge. Highly biocompatible, artificial systems consisting of all-aqueous, compartmentalized multicellular systems have yet to be realized. Here, a rapid multilevel compartmentalization of an all-aqueous system where a 3D sheet of subcolloidosomes encloses a mother colloidosome by interfacial phase separation is demonstrated. These spatially organized multicellular structures are termed "blastosomes" since they are similar to blastula in appearance. The barrier to nanoparticle assembly at the water-water interface is overcome using oppositely charged polyelectrolytes that form a coacervate-nanoparticle-composite network. The conditions required to trigger interfacial phase separation and form blastosomes are quantified in a mapped state diagram. We show a versatile model for constructing artificial multicellular spheroids in all-aqueous systems. The rapid interfacial assembly of charged particles and polyelectrolytes can lock in nonequilibrium shapes of water, which also enables top-down technologies, such as 3D printing and microfluidics, to program flexible compartmentalized structures.
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