Dynamically populating triplet excitons under external stimuli is desired to develop smart optoelectronic materials, but it remains a formidable challenge. Herein, we report a resonance-induced excited state regulation strategy to dynamically modulate the triplet exciton population by introducing a self-adaptive N-C═O structure to phosphors. The developed phosphors activated under high-power ultraviolet irradiation exhibited enhanced photoactivated organic ultralong room temperature phosphorescence (PA-OURTP) with lifetimes of up to ∼500 ms. The enhanced PA-OURTP was ascribed to activated N-C═O resonance variation-induced intersystem crossing to generate excess triplet excitons. The excellent PA-OURTP performance and ultralong deactivation time under ambient conditions of the developed materials could function as a reusable recorded medium for time-sensitive information encryption through optical printing. This study provides an effective approach to dynamically regulating triplet excitons and offers valuable guidance to develop high-performance PA-OURTP materials for security printing applications.