The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adom.202202382.the stored excitation energy in energy traps, which can be released by thermal stimulation. [2] Obviously, the process is very different from the real-time excited fluorescence (FL). Usually, the excitation source can be X-ray, ultraviolet (UV), and visible (Vis) light, and there is no need for continuous external light irradiation, while the PL may locate in UV, Vis, or near-infrared (NIR) spectral regions. [3] Especially, Vis emissions are easy to be modulated for colorful light, and NIR emissions in the biological window (≈650-1800 nm) offer deep tissue penetration and prevented autofluorescence. [3a,4] According to the outstanding luminescent properties, enormous opportunities in diverse application fields have been discovered, mainly including long-lasting tumor optical imaging and therapy, [5] security and anti-counterfeiting, [6] optical information and data storage, [7] photocatalysis, [8] fingerprint recognition, [6c] analysis and sensing, [1c,4a,9] as well as the potential applications of synaptic plasticity [10] and light-emitting diodes. [11] Retrieved from Web of Science, > 6800 articles by tracing the themes "afterglow" or "persistent luminescence" or "longlasting luminescence" have been published during the last decade (i.e., ≈2012-2022). Diverse categories of persistent luminescent materials have been developed, such as organic materials, [12] carbon dots, [13] metal-organic frameworks, [14] doped inorganic crystals et al. [2,15] Among them, organic afterglow materials, usually named as organic room temperature phosphorescence materials have recently drawn extensive attention due to the advantage of sustainable resources, low cost, and safety. [16] Based on the composition, organic afterglow materials can be mainly divided into organic small molecules, polymers, and organic-inorganic hybrids, which are normally related to the radiative transition from the lowest excited triplet state (T 1 ) to the ground state (S 0 ). Thus, methods for enhancing the intersystem crossing (ISC) rate are reasonable for realizing highly efficient afterglow, such as introducing heavy atoms, paramagnetic molecules, aromatic carbonyls, heteroatoms, and crystal engineering. [17] Recently, organic room-temperature phosphorescence with a high quantum yield above 56% and long afterglow lifetime longer than 22 s has been achieved by using suitable inorganic framework. [18] Additionally, color-tunable