This talk will address the development of principles that permit spatial and temporal control of molecular self-assembly in solution via the use of surfactants that incorporate the redox-active group called ferrocene. These surfactants, when combined with electrochemical and chemical methods, permit reversible control over a range of surfactant-based properties of solutions, including formation of micelles, solubilization of small molecules, formation of surfactant-polymer and surfactant-DNA complexes, and surface activity. This talk will introduce the fundamental molecular characteristics of this class of surfactants, and then illustrate how spatial and temporal control of oxidation state can be exploited to actively control the properties of these surfactant systems over a range of length and time scales. The presentation will focus on two examples. The first example will revolve around the generation of spatial gradients in surfactant concentration within microfluidic systems, thus realizing micrometer-scale gradients and patterns in micelle populations. Generation of spatially-constrained micelle populations on micrometer-scales will be shown to provide new means to manipulate driving forces for selective transport of molecular, macromolecular and mesoscopic species. The second case study will focus on temporal control over surfactant-biomolecule interactions, using DNA as an example of a biological macromolecule. Opportunities related to separations, drug delivery and sensing will be addressed.