A process is provided for precise self-assembly and re-arrangement of a three-dimensional terpyridine-based coordination complex. A plurality of terpyridine-containing ligands are reacted with at least one metal ion, in a pre-selected molar ratio, to form a self-assembled three-dimensional terpyridine-based coordination complex having a first configuration. A triggering event, such as exposure to light or dilution, causes the coordination complex to re-arrange to form at least two smaller, substantially identical, three-dimensional terpyridine-based coordination complexes, each having a second configuration that is different from the first configuration. Upon application of a second triggering event, such as concentration, the re-arrangement is reversed.