Organic ultralong room temperature phosphorescence (OURTP) materials having stimuli-responsive attributes have attracted great attention due to their great potential in a wide variety of advanced applications. It is of fundamental importance but challengeable to develop stimuli-responsive OURTP materials, especially such materials with modulated optoelectronic properties in a controlled manner probably due to the lack of an authentic construction approach. Here, we propose an effective strategy for OURTP materials with controllably regulated stimuli-responsive properties by engineering the resonance linkage between flexible chain and phosphor units. A quantitative parameter to demonstrate the stimuli-responsive capacity is also established by the responsivity rate constant. The designed OURTP materials demonstrate efficient photoactivated OURTP with lifetimes up to 724 ms and tunable responsivity rate constants ranging from 0.132 to 0.308 min-1 upon continuous UV irradiation. Moreover, the applications of stimuli-responsive resonance OURTP materials have been illustrated by the rewritable paper for snapshot and Morse code for multiple information encryption. Our works, which enable the accomplishment of OURTP materials capable of on-demand manipulated optical properties, demonstrate a viable design to explore smart OURTP materials, giving deep insights into the dynamically stimuli-responsive process.