Blue/deep-blue emission is crucial for organic optoelectronics but remains a formidable challenge in organic afterglow due to the difficulties in populating and stabilizing the high-energy triplet excited states. Here, a facile strategy to realize the efficient deep-blue organic afterglow is proposed via host molecules to sensitize the triplet exciton population of guest and water implement to suppress the non-radiative decays by matrices rigidification. A series of highly luminescent deep-blue (405–428 nm) organic afterglow materials with lifetimes up to 1.67 s and quantum yields of 46.1% are developed. With these high-performance water-responsive materials, lifetime-encrypted rewritable paper has been constructed for water-jet printing of high-resolution anti-counterfeiting patterns that can retain for a long time (>1 month) and be erased by dimethyl sulfoxide vapor in 15 min with high reversibility for many write/erase cycles. These results provide a foundation for the design of high-efficient blue/deep-blue organic afterglow and stimuli-responsive materials with remarkable applications.
