Multifunctional Amino‐Boranes Isomer Room‐Temperature Phosphorescent Material: Multi‐Substrate Multicolor Luminescence, Multi‐Level Anti‐Counterfeiting, Light‐Controlled Data Erasing/Writing, Data Logic Operation, and High Anti‐Laundry Detergent Performance.

Significant advances are made in understanding the structure‐property relationship in room‐temperature phosphorescence (RTP) materials. For example, intramolecular charge transfer (ICT) structural molecules based on electron donors(D) and electron acceptors(A) are an efficient method to achieve RTP. However, the ability to precisely regulate the singlet‐triplet energy gap (Δ<italic>E</italic>ST) through molecular design to control RTP emissions remains constrained. Herein, a group of <bold>4BN‐NP</bold> and <bold>5BN‐NP</bold> isomers is reported with D and A position isomerization, where <bold>4BN‐NP</bold> exhibits a photo‐induced orange afterglow phenomenon in PMMA. Calculations show that the spin‐orbit coupling (SOC) value of <bold>4BN‐NP</bold> is greater compared to <bold>5BN‐NP</bold> and the intersystem crossing (ISC) channel is more efficient, resulting in a smaller Δ<italic>E</italic>ST value for <bold>4BN‐NP</bold>. This indicates that the short ICT channel is more conducive to inducing phosphorescence emission. In addition, compound <bold>4BN‐NP</bold> co‐doped with red fluorescent dyes (RhB, Rh6G, and RBNN) in PMMA produces phosphorescence resonance energy transfer (PRET), inducing red afterglow emission. Surprisingly, light‐activated yellow RTP can be obtained by attaching <bold>4BN‐NP</bold> with polymethyl methacrylate (PMMA) to nylon filaments, and its phosphorescence intensity does not diminish even when it is immersed in water containing detergent solution, thus expanding the prospects of its application in textile encryption. [ABSTRACT FROM AUTHOR]