Evolution of Supramolecular Coordination Assemblies Visually Monitored by Time‐Dependent Multicolor Fluorescence

Abstract Supramolecular coordination assemblies play an important role in both material science and biological systems. Despite significant efforts in their development, most existing examples are thermodynamically controlled, which lack the adaptability and autonomy essential for the creation of advanced materials. In this work, we have developed non‐equilibrium coordination assembly systems that can evolve over time through a combination of thermodynamic and kinetic controls. The introduction of zinc ions resulted in the formation of metastable fiber assemblies in a kinetically trapped state, which autonomously converted to thermodynamically stable nanosheets over time. This evolution process can be regulated by external stimuli and visually monitored by the time‐dependent multicolor fluorescence. The construction strategy was versatile across other various ions such as Ca 2+ , Mg 2+ , and Al 3+ , offering inspiring insights for the design of complex systems that operated both in and out of their thermodynamic equilibrium.