anticounterfeiting, [1] sensing, [2] biological imaging, [3] logic encryption, [4] fingerprint recognition, [5] and organic light-emitting devices (OLEDs). [6] Recently, the exploitation of organic luminophores with RTP features has rapidly emerged as a hot research topic. They offer dramatic advantages of flexibility, simplicity of processing, high plasticity, outstanding biodegradability, good processability, and low cost, demonstrating widespread application prospects. With constant efforts of researchers, a series of corresponding methods have been proposed for approaching RTP nature, such as heavy atom effect, [7] H-aggregation, [8] hostguest doping, [9] and crystallization. [10] In contrast to the fluorescence, phosphorescence is generated from a much slower spin-prohibition transformation process from the triplet excited state to the singlet ground state. Thus, some triplet excited states of organic molecules or molecular aggregates are very susceptible to external stimuli, involving light, oxygen, pH, pressure, and so on. [11] The stimuli response properties of organic RTP materials have been employed to develop new approaches for information storage, sensors, and data encryption. [12] Among the organic RTP materials with stimuli response characteristics, photo irradiation-induced RTP materials are a class of unique functional carriers for constructing highperformance sensing and anticounterfeiting technologies. [13] However, the ambiguous inherent mechanisms and immature guidance for molecular design strategies limit the development of irradiation-induced RTP materials and their applications. In this context, we have attempted to utilize a simple building block for the construction of an organic RTP crystal with an irradiation-responsive feature. The simple system is beneficial to deeply understand the mechanism of irradiation-induced RTP and further extend its material system.