This presentation will describe approaches leading to reversible control over the self-assembly of surfactants at interfaces and in bulk solution. The approaches are based on the use of redox-active and light-responsive surfactants. When combined with electrochemical and photochemical methods, these surfactants permit spatial control over self-assembly processes as well as provide ways to generate well-defined gradients in properties of aqueous surfactant systems. This talk will sketch dynamic and equilibrium properties of these novel surfactant systems, and illustrate potential uses of these surfactants in processes and technologies, including micro-scale mixing, separations and biotechnology.