Biomineralization‐Inspired Membranization Toward Structural Enhancement of Coacervate Community

Abstract The design and assembly of protocell models that can mimic the features and functions of life present a significant research challenge with the potential for far‐reaching impact. Inspired by the natural phenomenon of microbe‐induced mineralization, a way is developed to induce the spontaneous formation of mineralized membrane on the surface of coacervate droplets utilizing Fe 3+ ions. In particular, the effect of Fe 3+ ions on the microstructure of droplets at the molecular level is dissected by combining theoretical and experimental approaches. The reversible formation process of membrane can be regulated by redox reactions involving Fe 2+ /Fe 3+ ions within the coacervate. The formation of mineralized membrane not only enhances the stability of the coacervate droplets and prevents aggregation and coalescence, but also allows the aggregation of adjacent droplets together. The membranized coacervate assemblages retain the inherent properties of biomolecule sequestration and enzyme catalysis, and also demonstrate excellent resistance to high temperatures and pressures as well as good stability for over 30 days. This study will offer a new platform for the assembly of coacervate‐based life‐like biomimetic systems, as well as enhance the understanding of the interactions underlying various biological phenomena at the molecular level.