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Liquid–liquid phase separation of macromolecules is an important process in many biological and synthetic systems. The process results in the formation of coacervates that act as membraneless compartments for storage and concentrated polymer precursors to solid phase materials. Here, we present a general strategy to form coacervates from nonionic block copolymers by controlling the molecular structure and solvent composition. The mechanism of coacervation is studied using a combination of optical microscopy and cryogenic and liquid phase electron microscopy, revealing a coalescence-driven growth process. Knowledge of the mechanism enables the design of experiments where morphological information is encoded into the coacervate phase and developed into the solid phase. The results show that self-assembled materials can be formed with multiple morphologies from the nanoscale up to the …