Spray synthesis is ar obustr oute to compositionally complex materials as fine powders;h owever,t he solidstate synthetic conditions in most cases limit access to discrete nanoparticles with defined structural features. Yet, by maintaining ad ynamic droplet phase through integration of molten salt chemistry,p roduct formation can proceed in manners similart ol ower temperature solution routes to nanomaterials. This Focus Review connects concepts from classical nucleation theory and molten salt chemistry to provide af ramework for nanocrystal formation via aerosol-assisted molten salt synthesis (AMSS). Examples of metal oxide nanocrystal formation by AMSS are surveyed and highlight how the spatiala nd temporal confinement of aerosold roplets limits crystal growth in molten media. Ultimately,w e strive to provide practical guidelines, not limited to AMSS, towardst he synthesis of compositionally complex materials as shape-defined nanocrystals.