The stimulus-responsive behavior of an adsorbed monolayer of diblock copolymer micelles was described. The reversible layer reconstructions that require no drying and/or annealing processes or the use of organic solvents were also demonstrated. Diblock copolymers can associate or dissociate in bulk solution in response to biologically significant stimuli as solution pH, ionic strength, and temperature. A significant change was revealed in the morphology of the adsorbed copolymer layer in response to pH cycling. It was also found that smart surfaces could be exploited for targeted encapsulation and/or release applications that require multiple recycling and/or reversibility.