Supramolecular polymers have attracted considerable interest due to their intriguing features and functions. The dynamic reversibility of noncovalent interactions endows supramolecular polymers with tunable physicochemical properties, self-healing, and externally stimulated responses. Among them, pillararene-based supramolecular polymers show great potential for biomedical applications due to their fascinating host–guest interactions and easy modification. Herein, we summarize the state of the art of pillararene-based supramolecular polymers for cancer therapy and illustrate its developmental trend and future perspective.