AbstractSupramolecular structures assembled via noncovalent interactions have found diverse applications in mechanical, biological, electronic, and manufacturing‐related fields. Ionic interactions represent key noncovalent interactions, which can be used, for example, to create highly ordered, responsive, conductive, reversible, and/or viscoelastic supramolecular assemblies. The recent advances in the field of ionic supramolecular assemblies, including those prepared from polymers, small molecules, or a combination of the two are reviewed. The versatility and simplicity of constructing ionic supramolecular assemblies are illustrated through several examples. Finally, the outstanding issues and potential opportunities are discussed to stimulate critical discussions and encourage further discovery.