Abstract: Non-covalent cross-linking interactions can be used to tailor stiffness and strength of linear polymers while enabling interesting features like self-healing, energy dissipation, and extended stretching capability. Metallopolymers in particular are highly customizable since in addition to normal polymer control knobs such as monomer selection, molecular weight and architecture, metallopolymers can be differentiated by the type of metal cation, ligand chemistry on the polymer, and the addition of non-covalently bonded ligands. In this talk I will present key aspects of my group’s work towards tailoring otherwise linear polymers with metal cation-based crosslinks. Our goal throughout is to explicitly connect the macroscale observed mechanical properties to the mechanics and dynamics of the metal cation-based crosslinks. Consequently, this work spans many approaches including synthesis, experiments, rheological modeling, and density functional theory. I will also share brief highlights from ongoing material design projects in our group at larger length scales.