Trap Depth Modulation and Antenna Effect of Organic Ligands for Enhancing Rare‐Earth Long Persistent Luminescence

Rare‐earth long persistent luminescence (LPL) materials with unique light‐storage properties show great promise for diverse applications. However, modifying the optical properties of such materials is extremely challenging due to their inherent characteristics. Here, we propose a coordination modification strategy that not only deepens the trap depth but also enhances the light‐capturing capability of rare‐earth LPL materials by introducing organic ligands as an antenna. Unlike previous single‐case demonstrations, this strategy is systematically validated across multiple LPL hosts with different afterglow colors, including green (SrAl 2 O 4 :Eu 2+ , Dy 3+ ), red (Sr 0.75 Ca 0.25 S:Eu 2+ ), and blue (SrSiO 3 :Eu 2+ , Dy 3+ ). Experimental results demonstrate that the afterglow intensity, brightness, and duration of the organic–inorganic hybrid LPL materials have been significantly enhanced compared to the original LPL materials. Based on this performance breakthrough, we further demonstrate the application potential of these materials in diverse scenarios, including flexible displays, intelligent sensors, and multi‐level information encryption. This work not only provides an efficient method for enhancing the performance of multi‐color long persistent luminescence materials but also offers new design insights for developing novel organic–inorganic hybrid luminescent systems.