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Recent booming advances in luminescent gold nanoclusters (AuNCs), have prompted the development of novel fluorescent sensors. The luminescent AuNCs possess unique and intriguing physical and chemical properties including responsive photoluminescence and peroxide-like activity, providing abundant potentials for sensing strategy design. As of now, a wide variety of chem-/bio-sensors based on AuNCs have been developed and reviewed according to varied analytes. In this review, from a different point of view, we follow the route of how those sensors realize their functions and focus on the actual roles AuNCs play, in order to hierarchically and logically display the recent progress in the sensing applications of AuNCs. This review not only opens new windows to understand the development of sensors based on AuNCs but can also inspire broader and deeper utilization of luminescent nanomaterials.