Abstract: The methods of the invention employ electrostatic atomization to form a compound droplet of at least two miscible fluids. The compound droplet comprises a core of a first fluid and a layer of a second fluid completely surrounding the core. The first fluid contains the agent to be encapsulated and the second fluid contains an encapsulating agent. The first and second liquids are miscible. The encapsulated droplets can contain a variety of materials including, but not limited to, polynucleotides such as DNA and RNA, proteins, bioactive agents or drugs, food, pesticides, herbicides, fragrances, antifoulants, dyes, oils, inks, cosmetics, catalysts, detergents, curing agents, flavors, fuels, metals, paints, photographic agents, biocides, pigments, plasticizers, propellants and the like and components thereof. The droplets can be encapsulated by a variety of materials, including, but not limited to, lipid bilayers and polymer shells.