Hierarchical Assembly of Proteinosomes and Coacervates Communities into 3D Protocellular Networks

Drawing inspiration from the living cells, various life‐inspired assemblies have been developed to mimic their remarkable properties and functionalities, and offer valuable insights into the origin of life and the understanding of life behaviors. Advancing the design and construction of multi‐compartmentalized hierarchical systems with more advanced structures and functions has always increasingly attracted attention in this field. Here, a type of 3D protocellular networks are designed and constructed, which is formed by the hybrid of two types of protocells communities based on phenylboronic acid‐grafted proteinosomes and polysaccharide‐based coacervate microdroplets. Progressive self‐assembly process is investigated to understand their characteristics and functions, including the host‐guest self‐assembly, the multi‐compartmentalized hierarchical self‐assembly, and bulk aqueous self‐assembly. Notably, the 3D protocellular networks‐based bulk condensate phase, which is bulk aqueous self‐assembled by physical support between vesicles‐ and droplets‐based protocells communities, exhibit the regulation of enzymatic reactions based on the enzyme enrichment and adhesiveness of the condensate phase. The results establish a platform for investigating the interactions between protocell communities and provide opportunities for the fabrication of functional 3D protocellular networks with a new view to engineer biomimetic prototissues.