Coacervate droplets are promising microcompartments for mimicking complex, life-like behavior. Autocatalytic reactions are at the basis of nonlinear reactions, such as chemical oscillations and self-replication. In this issue of Chem, Hanopolskyi et al. use the autocatalytic nonenzymatic guanidation of a polyamine to control the formation and structure of coacervates. Coacervate droplets are promising microcompartments for mimicking complex, life-like behavior. Autocatalytic reactions are at the basis of nonlinear reactions, such as chemical oscillations and self-replication. In this issue of Chem, Hanopolskyi et al. use the autocatalytic nonenzymatic guanidation of a polyamine to control the formation and structure of coacervates. Interplay between autocatalysis and liquid-liquid phase separation produces hierarchical microcompartmentsHanopolskyi et al.ChemSeptember 28, 2023In BriefComplex coacervates are important for intracellular functions and as prebiotic compartments in the search for the origin of life. In this work, Hanopolskyi et al. obtained complex coacervates in an autocatalytic reaction. Interestingly, the reaction produced biphasic hierarchical microcompartments when oil droplets were formed in addition to coacervate droplets. The sigmoidal profile of the autocatalytic reaction kinetically controls the assembly process. The authors demonstrated the application of this mechanism for synthesizing complex compartments from desired phases. Full-Text PDF