Supramolecular polymers allow access to dynamic materials, where noncovalent interactions can be used to offer both enhanced material toughness and stimuli-responsiveness. The versatility of self-assembly has enabled these supramolecular motifs to be incorporated into a wide array of glassy and elastomeric materials; moreover, the interaction of these noncovalent motifs with their environment has shown to be a convenient platform for controlling material properties. In this Viewpoint, supramolecular polymers are examined through their self-assembly chemistries, approaches that can be used to control their self-assembly (e.g., covalent cross-links, nanofillers, etc.), and how the strategic application of supramolecular polymers can be used as a platform for designing the next generation of smart materials. This Viewpoint provides an overview of the aspects that have garnered interest in supramolecular polymer chemistry, while also highlighting challenges faced and innovations developed by researchers in the field.