Nature is remarkably adept at using interfaces to build structures, encapsulate reagents, and regulate biological processes. Inspired by Nature, we describe flexible polymer-based ribbons, termed mesoscale polymers (MSPs), 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.
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