This study explores the design and application of dipeptide coacervates as artificial membraneless organelles for bioorthogonal catalysis. Coacervates, which are spontaneously formed liquid droplets, have emerged as promising biomimetic materials due to their molecular crowding and selective partitioning properties. However, their use as artificial organelles has been limited by complex molecular structures, limited control over internal microenvironments, and colloidal instability. The authors designed dipeptide coacervates with enhanced stability, biocompatibility, and a hydrophobic microenvironment, which facilitates the encapsulation of hydrophobic species, including transition metal-based catalysts. These coacervates were incorporated into cells as active artificial organelles, enabling non-biological chemical reactions within the cell. The development of coacervates with a hydrophobic microenvironment opens new avenues in biomimetic materials, particularly in catalysis and synthetic biology. The study demonstrates the potential of dipeptide coacervates as versatile and biocompatible microreactors for enhancing catalytic activity in water-based systems and enabling bioorthogonal reactions within living cells.This study explores the design and application of dipeptide coacervates as artificial membraneless organelles for bioorthogonal catalysis. Coacervates, which are spontaneously formed liquid droplets, have emerged as promising biomimetic materials due to their molecular crowding and selective partitioning properties. However, their use as artificial organelles has been limited by complex molecular structures, limited control over internal microenvironments, and colloidal instability. The authors designed dipeptide coacervates with enhanced stability, biocompatibility, and a hydrophobic microenvironment, which facilitates the encapsulation of hydrophobic species, including transition metal-based catalysts. These coacervates were incorporated into cells as active artificial organelles, enabling non-biological chemical reactions within the cell. The development of coacervates with a hydrophobic microenvironment opens new avenues in biomimetic materials, particularly in catalysis and synthetic biology. The study demonstrates the potential of dipeptide coacervates as versatile and biocompatible microreactors for enhancing catalytic activity in water-based systems and enabling bioorthogonal reactions within living cells.