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Significance There has been considerable interest in the construction of stimuli-responsive metallosupramolecular architectures because of their versatile structural and bonding properties, imparting them with the capability to exhibit specific functions. Despite a variety of metal–organic architectures reported, those involving noncovalent metal–metal interactions and luminescence changes that depend on the nature of the guests are rather underexplored. Herein, a series of alkynylplatinum(II) terpyridine molecular rectangles has been shown to exhibit reversible capture and release of anticancer therapeutic guests under different pH conditions with instant and drastic color and luminescence responses. The fundamental understanding of these host–guest interactions has led to the development of a unique proof-of-principle multiaddressable model system that illustrates the capability of reversible guest capture and release processes for therapeutic delivery.

Multiaddressable molecular rectangles with reversible host–guest interactions: Modulation of pH-controlled guest release and capture