The traditional construction of materials is usually driven by classical synthetic transformations involving the making and breaking of covalent bonds. These processes often require high energy input and highly reactive and hazardous materials. In natural systems, one typically encounters synthetic control schemes that are based on entropic forces rather than these human-designed enthalpic manipulations. In natural processes, phase changes and triggered mixing are often employed to direct systems towards or away from equilibrium conditions. The recognition of these "natural tendencies" allows one to design processes that have reduced toxicological and environmental impact. This presentation will describe results in non-covalent derivatization that illustrate this shift towards entropic control.