Immobilization of π-assembled metallo-supramolecular arrays in thin films: from crystal-engineered structures to processable materials

Layer‐by‐layer deposition of π‐assembled arrays of discrete metallo units with aryl tails and polystyrenesulfonate gives structurally well‐defined thin films (see schematic representation). The formation of these films, which is controlled by π–π interactions, metal–ion coordination, and electrostatic interactions, bridges the gap between supramolecular crystal engineering and design of layered materials.