| Summary: | Abstract Persistent mechanoluminescence (ML) with long lifetime is highly required to break the limits of the transient emitting behavior under mechanics stimuli. However, the existing materials with persistent ML are completely trap‐controlled, and a pre‐irradiation is required, which severely hinders the practical applications. In this work, a novel type of ML, self‐charging persistent ML, is created by compositing the Sr3Al2O5Cl2:Dy3+ (SAOCD) powders into flexible polydimethylsiloxane (PDMS) matrix. With no need for any pre‐irradiation, the as‐fabricated SAOCD/PDMS elastomer could exhibit intense and persistent ML under mechanics stimuli directly, which greatly facilitates its applications in mechanics lighting, displaying, imaging, and visualization. By investigating the matrix effects as well as the thermoluminescence, cathodoluminescence, and triboelectricity properties, the interfacial triboelectrification‐induced electron bombardment processes are demonstrated to be responsible for the self‐charged energy in SAOCD under mechanics stimuli. Based on the unique self‐charging processes, the SAOCD/PDMS further exhibits mechanics storage and visualized reading activities, which brings novel ideas and approaches to deal with the mechanics‐related problems in the fields of mechanical engineering, bioengineering, and artificial intelligence.
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