Reactions Coupled Self‐ and Co‐Assembly: A Highly Dynamic Process and the Resultant Spatially Inhomogeneous Structure

Abstract Reactions coupled self‐assembly represents a step forward towards biomimetic behavior in the field of supramolecular research. Here, two pH‐dependent reactions of thiol‐disulfide exchange and ligand exchange were used to couple with the self‐assembly of an AuI‐thiolate coordination polymer consisting of two ligands. Thanks to the comparable rates between the reactions and self‐assembly, the compositions of the assemblies change continuously with time, resulting in a highly dynamic assembly process and spatially inhomogeneous structure that are very common in life systems but cannot be easily obtained with one‐pot artificial methods.