Mechanoluminescent materials have shown great application potential in the fields of stress detection, anticounterfeiting, and optical storage; however, its development is hindered by the unclear mechanism. Different from the mainstream exploration of new mechanoluminescent materials in noncentrosymmetric structures, a centrosymmetric mechanoluminescent material Li 2 ZnGeO 4 :Mn 2+ is synthesized by a standard hightemperature solid-state reaction in an ambient atmosphere. Combined with the Rietveld refinement, photoluminescence, electron spin resonance, and X-ray photoelectron spectroscopy, it is proved that the increase in oxygen vacancies is accompanied by the self-reduction process from Mn 4+ to Mn 2+ , and the mechanism of mechanoluminescence is clarified through the afterglow and thermoluminescence spectra. The carriers trapped by the shallow traps participate in the mechanoluminescence process through the tunneling effect, while the carriers trapped by the deep traps take part in the mechanoluminescence process via conduction band or tunneling. A signature anti-counterfeiting application is designed using the new mechanoluminescent material Li 2 ZnGeO 4 :0.004Mn 2+ . Utilizing the afterglow characteristics of Li 2 ZnGeO 4 :xMn 2+ phosphors, we designed an intelligent longpersistent luminescence quick response code (QR-code) and visualized information encoding/decoding model, which provides a fast, simple, and effective method for information encryption, transformation, and dynamic anti-counterfeiting. This study not only analyzes the self-reduction and mechanoluminescence processes in detail but also breaks the limitation of crystal symmetry and provides a new strategy for the exploration of novel mechanoluminescent materials.