Metallo-supramolecular polymers (MSPs) have emerged as a dynamic field in soft materials and nanomaterials over the past three decades. The unique interplay of ligands and metal ions plays a crucial role in defining their properties, such as binding strength and topology, making these systems distinct from their all-organic counterparts. Furthermore, the incorporation of metal centers introduces redox activity, unique photophysical properties, and electronic functionality. As a result, these systems can exhibit stimuli-responsive behavior, essential for applications in optoelectronics and biology. However, challenges remain in achieving precise control over self-assembly, morphology, and spatiotemporal responsiveness, as well as a clear rationale between coordination and self-assembly behavior. Our review, therefore, summarizes recent advances in ligand design, coordination modulation, and polymerization techniques, offering new strategies to rationally develop MSPs with tailored functionalities.
