Evolving Emulsion Microcompartments via Enzyme‐Mimicking Amyloid‐Mediated Interfacial Catalysis

Abstract Living organisms take in matter and energy from their surroundings, transforming these inputs into forms that cells can use to sustain metabolism and power various functions. A significant advancement in the development of protocells and life‐like materials has been the creation of cell‐like microcompartments capable of evolving into higher‐order structures characterized by hierarchy and complexity. In this study, a smart emulsion system is designed to digests chemical substrates and generates organic or inorganic products, driving the self‐organization and structuration of microcompartments. Central to this system is a lipase‐derived peptide that undergoes amyloid fibrillation, exhibiting hydrolase‐like activity and stabilizing Pickering emulsions. Through catalytic hydrolysis or silicatein‐inspired mineralization, these emulsion microcompartments generate self‐organized surfactant layers from organic substrates or silica scaffolds from inorganic substrates at the oil–water interface, respectively, helping to prevent coalescence. This process further facilitates a structural evolution into high‐internal phase emulsion gels that are suitable for direct‐ink‐writing 3D printing. The findings underscore the potential for designing self‐evolving soft materials that replicate the structures and functions of living organisms.