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Abstract An active droplet system, programmed to repeatedly move autonomously at a specific velocity in a well‐defined direction, is demonstrated. Coulombic energy is stored in oversaturated interfacial assemblies of charged nanoparticle‐surfactants by an applied DC electric field and can be released on demand. Spontaneous emulsification is suppressed by an increase in the stiffness of the oversaturated assemblies. Rapidly removing the field releases the stored energy in an explosive event that propels the droplet, where thousands of charged microdroplets are ballistically ejected from the surface of the parent droplet. The ejection is made directional by a symmetry breaking of the interfacial assembly, and the combined interaction force of the microdroplet plume on one side of the droplet propels the droplet distances tens of times its size, making the droplet active. The propulsion is autonomous, repeatable, and agnostic to the chemical composition of the nanoparticles. The symmetry‐breaking in the nanoparticle assembly controls the microdroplet velocity and direction of propulsion. This mechanism of droplet propulsion will advance soft micro‐robotics, establishes a new type of active matter, and introduces new vehicles for compartmentalized delivery.