LAUSR

Exploring efficient strategies to enhance persistent luminescence (PersL) is highly demanded to facilitate advanced applications of inorganic PersL phosphors. In this work, a remarkable enhancement of Mn2+ PersL in LiYGeO4 (LYGO) with tunable wavelengths is achieved through Bi3+ codoping. The Mn2+ emission can be tuned from 600 to 664 nm by increasing the doping concentration, attributed to site‐selective occupation of different crystallographic sites. The pronounced enhancement in the PersL of Mn2+ is achieved through the synergistic interplay of energy transfer from Bi3+ to Mn2+ and electron‐capture competition between the two hole‐trapped ions. Specifically, the PersL intensity of LYGO:0.5%Mn2+,0.125%Bi3+ at 30 s increased by 444 times compared to that of LYGO:0.5%Mn2+ after 254 nm excitation. Thermoluminescence measurement reveals that introduction of Bi3+ creates an additional trap center with depth of 0.60 eV. Moreover, LYGO:Mn2+,Bi3+ exhibits excellent water resistance and shows great potential for applications in information storage and X‐ray detection. This work not only demonstrates an intense red PersL phosphor, but also provides an efficient strategy to enhance PersL in inorganic materials via energy transfer and electron‐capture competition.