AlN is a core material widely used as a substrate and heat sink in various electronic and optoelectronic devices. Introducing luminescent properties into intrinsic AIN opens new opportunities for next‐generation intelligent sensors, self‐powered displays, and wearable electronics. In this study, the first evidence is presented of AlN crystals exhibiting satisfactory mechanoluminescence (ML), photoluminescence (PL), and afterglow performance, demonstrating their potential as novel multifunctional optical sensors. A series of undoped AlN crystals (ranging from µm to mm scale) is successfully synthesized on tungsten substrates via physical vapor transport. A multimodal optical sensing platform is developed, showing afterglow and PL for temperature and pressure sensing, and ML for force detection. Despite minimal structural deformation under extreme conditions, attributed to the high bulk modulus of AIN, the optical …