Supramolecular chemistry has been used to tackle some of the major challenges in modern science, including cancer therapy and diagnosis. Supramolecular platforms provide synthetic flexibility, rapid generation through self-assembly, facile labelling, unique topologies, tunable reversibility of the enabling noncovalent interactions, and opportunities for host–guest chemistry and mechanical bonding. In this Review, we summarize recent advances in the design and radiopharmaceutical application of discrete self-assembled coordination complexes and mechanically interlocked molecules — namely, metallacages and rotaxanes, respectively — as well as in situ-forming supramolecular aggregates, specifically pinpointing their potential as next-generation radiotheranostic agents. The outlook of such supramolecular constructs for potential applications in the clinic is discussed.

超分子化学已被用于解决现代科学中的一些主要挑战，包括癌症治疗和诊断。超分子平台提供合成灵活性、通过自组装快速生成、简单的标记、独特的拓扑结构、使能非共价相互作用的可调可逆性，以及主客体化学和机械键合的机会。在这篇综述中，我们总结了离散自组装配位复合物和机械互锁分子（即金属溶隙和轮烷）以及原位形成的超分子聚集体的设计和放射性药物应用的最新进展，特别指出了它们作为下一代放射热麻醉剂的潜力。讨论了这种超分子构建体在临床上的潜在应用的前景。