Near-infrared (NIR) mechanoluminescent materials are attracting significant attention due to their potential applications in biomedical imaging, food analysis, and night vision. In this study, Tb₃Al₅O₁₂:Cr³⁺(TAG:Cr³⁺) phosphors were successfully synthesized using a conventional high-temperature solid-state method. These materials demonstrated enhanced NIR luminescence through energy transfer (ET) between Tb³⁺ and Cr³⁺. The structural and luminescent properties of the TAG:Cr³⁺ phosphors were systematically investigated, revealing a strong spectral overlap between the emission of Tb³⁺ and the excitation of Cr³⁺, which facilitates efficient ET. When embedded in polydimethylsiloxane (PDMS) composites, the phosphors exhibited notable mechanoluminescence (ML) properties, showing robust response and recoverability under repeated mechanical stimulation. Density functional theory (DFT …