Programmed Wrapping and Assembly of Droplets with Mesoscale Polymers

Nature is remarkably adept at using interfaces to build structures, encapsulate reagents, and regulate biological processes. Inspired by nature, flexible polymer‐based ribbons, termed “mesoscale polymers” (MSPs), are described to modulate interfacial interactions with liquid droplets. This produces unprecedented hybrid assemblies in the forms of flagellum‐like structures and MSP‐wrapped droplets. Successful preparation of these hybrid structures hinges on interfacial interactions and tailored MSP compositions, such as MSPs with domains possessing distinctly different affinity for fluid–fluid interfaces as well as mechanical properties. In situ measurements of MSP–droplet interactions confirm that MSPs possess a negligible bending stiffness, allowing interfacial energy to drive mesoscale assembly. By exploiting these interfacial driving forces, mesoscale polymers are demonstrated as a powerful platform that underpins the preparation of sophisticated hybrid structures in fluids.