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Near‐infrared (NIR) long‐persistent phosphors (LPPs) have emerged as a potential solution for bio‐imaging applications over the past few years. However, there are enormous challenges regarding their in situ application based on their dependence on short‐wavelength excitation. In this paper, we report a multi‐spectral excited NIR LPP, Li5Zn8Ga5Ge9O36: 1.5 % Cr3+, 0.5 % Ti4+, which overcomes the limitations of functional processes in biological tissues and other complex systems. This LPP exhibits a high luminescent intensity and a long emission duration in the NIR region (700–800 nm). The applicability of this phosphor to tissue imaging is demonstrated experimentally. Its persistent luminescence (PersL) can easily penetrate approximately 2 mm of pork flesh. More importantly, this phosphor can be re‐charged in situ using a red LED or laser diode array to provide renewed NIR PersL for biological tissues, which is beneficial for long‐term biological tissue imaging applications with high signal‐to‐noise ratios. Systematic investigations of the nature of energy traps and PersL mechanisms are also reported in this paper.

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