Molecular motor-driven reversible liquid-liquid phase separation of supramolecular assemblies.

Liquid-liquid phase separation (LLPS) is a crucial process in natural and artificial systems, capable of maintaining cellular behavior and realizing material functions. While supramolecular assemblies provide a versatile platform for understanding natural phenomena and developing adaptive materials, their LLPS remains largely unexplored, particularly with respect to reversible control. Here, we report a molecular motor-driven LLPS system, where nanoscale rotary motion modulates LLPS of supramolecular assemblies. Systematic molecular modification and photothermal isomerization studies comprehensively reveal that subtle changes in molecular structure affect the hydrophobicity of molecules, which in turn decrease the critical phase separation temperature and promotes the phase separation. During the rotary of molecular motor, these assemblies undergo in situ formation and dissolution of droplets across multiple non-equilibrium states. Our findings establish an orthogonal strategy to tune phase separation by light and temperature, providing an avenue for designing out-of-equilibrium biomedical materials and adaptive soft matter systems.