Self-assembled organic ligand functionalized microcapsules encapsulating one or more substrates, which release the substrates upon activation with a power source, are provided. Compositions that include these microcapsules, as well as methods of making the microcapsules and releasing the encapsulated substrates are also provided. The structures, compositions and methods find use in a variety of applications, such as drug and cell encapsulation technologies, for direct delivery, control, and activation of medicines and therapies to specific tissues in a living host e.g. targeted cancer therapy and pain management.