Microcompartments with Strong and Dynamic Self‐Repairing Shells

Abstract Microcompartments are useful for the storage, controlled reaction, and release of active compounds. However, the useful lifetime of a microcompartment is generally ended when it ruptures. Here, a self‐repairing microcompartment is proposed whose dynamic polymer shell can seal after rupturing, thus extending the lifetime of the capsule and allowing for multiple mechanically‐stimulated release events. The dynamic polymer shell is created in a one‐step approach through the formation of a double network polymer in the oil phase of a double emulsion template made by microfluidics. Of the two networks, a permanently‐crosslinked network is introduced to elastically restore the shape of the microcompartment, while a dynamically‐crosslinked network forms new bonds across crack interfaces. By quantifying the timescales required for the formation of new dynamic bonds within ruptured shells, strong microcompartments with predictable strength recovery and self‐repairing capabilities are successfully prepared and used to demonstrate the possibility of mechanically‐stimulated multiple release of cargo molecules.