Metal−organic frameworks (MOFs) represent an attractive family of materials for diverse biomedical applications due to their porosity, chemical versatility, and stimuli-responsive properties. Next to their drug delivery and bioimaging applications, MOFs have been recently considered as efficient luminescent thermal probes. However, the relatively low thermal sensitivity together with the biocompatibility of most MOF thermometers limits their practical applications. Here, a series of new MOFs based on Zn ions and a rectangular tetratopic ligand H