Cancer is one of the world's most serious health challenges. Several problems and challenges still exist for cancer therapies especially because anti-cancer agents that are delivered to normal cells and tissues cause a number of severe side effects. In one general approach aimed at solving this problem, supramolecular systems, created by noncovalent interactions, have been designed and utilized for cancer-cell-targeted drug delivery. In addition, cancer-associated, turn-on supramolecular theranostic agents have received great attention in the biomedicine field because they can be selectively ''switched on'' in cancer cells. This attribute enables the avoidance of problems associated with cytotoxic effects on healthy cells and tissues. In this review, we summarize recent progress made in the design of turn-on supramolecular theranostic agents composed of host-guest nanosystems and their applications in biomedicine.