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Electrostatic interactions can be used in the self-assembly of a wide range of responsive, bioinspired soft materials ranging from dehydrated thin films, fibers, and bulk solids to dense, polymer-rich liquid complex coacervates, as well as more complex hierarchical structures such as micelles and hydrogels. This responsiveness can include swelling and dissolution or solidification, which can be harnessed to facilitate encapsulation and the subsequent fabrication of functional materials. We draw inspiration from biomolecular condensates, which utilize liquid-liquid phase separation to create transient compartments in cells.