Mechanical Energy Drives Dissipative Self-Assembly of Nanocoacervates into Vesicles with Cell-like Properties.

Dissipative self-assembly, which relies on continuous energy input to form and sustain functional structures, underpins the adaptive behaviors of biological systems and is essential for creating synthetic materials with life-like properties. While chemical, thermal, photonic, or electrical energy sources have been used for dissipative self-assembly of nanostructures, this work pioneers mechanical energy as a novel driver to create dissipative polyelectrolyte micrometrical vesicles, with a half-life of ca. 2 days that exhibit cell-like properties such as selective molecular uptake and catalytic functionality. Our strategy works with different polyelectrolyte systems, including DNA and peptides, suggesting relevance to natural systems and the origins of life. Finally, we demonstrate that mechanical energy can also drive the evolution of distinct dissipative vesicle populations into a single, higher-order population with advanced compartmentalization and enhanced synthetic capabilities. Our work establishes mechanical energy as a key driver of dissipative self-assembly, with implications for life-like materials engineering, biotechnology, and microreactor design.