Abstract Here, we describe the recent progress on metal‐coordinated supramolecular structures with unique characteristics and controlled helicity based on coordination geometry and dynamic intermolecular binding events. The current major research area is the self‐assembly of a metal‐containing molecule into nanomaterials. It generated a large number of supramolecular polymers, which have various structures and functions. Although the dynamic coordination complexation reactions between various metal ions and ligands are spontaneous, we successfully achieved unique morphological transformations with helical inversion of metal‐containing supramolecular polymers via the kinetic control of dynamic coordination complexation reactions. Our findings have a significant impact on the development of novel and advanced supramolecular materials, and dynamic coordination bonds in the molecular design of metal‐containing complexes for modulating self‐assembly pathways, which may be relevant for the fabrication of supramolecular materials with interesting properties. Our contributions may be useful to the understanding of chiral assembly processes in biological systems.