Conclusion and Outlook Noncovalent interactions, being fundamental in nature, dictate various biological processes. While the tunability and versatility of noncovalent interactions are well-established for generating supramolecular biomaterials as potential biomedicine, the precise control of the reversibility of noncovalent interactions is not only a unique advantage, but also an unmet challenge. The complex and dynamic cellular environment changes noncovalent interactions constantly, making it hard to predict the behavior of supramolecular biomaterials in vivo. Various enzymes may also deactivate biomaterials before they reach effective sites. Besides, supramolecular biomaterials require a minimum concentration to assemble, which is hard to maintain under several elimination pathways in vivo. Despite several aforementioned examples of supramolecular assemblies in biomedicine, the study of their applications is just beginning and much of the study remains to be carried out. Therefore, unravelling the mechanism of actions, and achieving spatiotemporal control in vivo are ultimate goals in developing biomedical applications of supramolecular biomaterials, such as modulating cellular processes and controlling cell fate. To address the unresolved challenges requires the cooperation from chemists, biologists, pharmacists, and engineers. This interdisciplinary research field continues to progress (Wang et al., 2020[89]; Yang et al., 2020[102]; Kim et al., 2020[42]; Xu et al., 2020[98]; Li et al., 2020[56]; Cheng et al., 2019[10][11]; Roy et al., 2020[71]) and to result in interesting discoveries for the years to come.