Owing to the rapid development of the nuclear industry, uranium has become a global environmental contaminant due to its radiotoxicity and chemotoxicity, posing significant threats to human health and ecological safety. Although various instrumental and chemical analytical methods have been developed for uranyl ion detection in aquatic environments, searching for new sensors with high stability, sensitivity, and selectivity remains a challenge. In this study, a luminescent Zr-based metal-organic framework (MOF), designated as Tb@UiO-66-(COOH)