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Mechanoluminescence, a smart luminescence phenomenon in which light energy is directly produced by a mechanical force, has recently received significant attention because of its important applications in fields such as visible strain sensing and structural health monitoring. Up to present, hundreds of inorganic and organic mechanoluminescent smart materials have been discovered and studied. Among them, strontium‐aluminate‐based materials are an important class of inorganic mechanoluminescent materials for fundamental research and practical applications attributed to their extremely low force/pressure threshold of mechanoluminescence, efficient photoluminescence, persistent afterglow, and a relatively low synthesis cost. This paper presents a systematic and comprehensive review of strontium‐aluminate‐based luminescent materials’ mechanoluminescence phenomena, mechanisms, material synthesis techniques, and related applications. Besides of summarizing the early and the latest research on this material system, an outlook is provided on its environmental, energy issue and future applications in smart wearable devices, advanced energy‐saving lighting and displays.

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