ConspectusStimuli-responsive materials have a great potential in various novel photoelectric devices, such as self-adaptive adjustment devices, intelligent detection, molecular computers with information storage capability, camouflage and anticounterfeiting display, various energy-saving displays, and others. However, progress in related areas has been relatively slow because of the lack of high-performance smart materials and the limitations of available reaction mechanisms currently. To address these problems fundamentally, new mechanisms need to be designed and developed, and learning from nature is an effective and intelligent method to achieve this long-awaited target, such as mimicking of proton transfer processes in nature at the molecular/supramolecular level. The stimuli-induced reversible proton transfer system is composed of materials that release or capture protons in response to stimuli and switch molecules that control color and/or fluorescence modulation by protons, and it is applied in stimuli-responsive materials and devices, including bistable electronic/electrochromic devices, electrofluorochromic devices, water-jet rewritable paper, visible-light-responsive rewritable paper, and mechanochromic materials.To help researchers gain deep insight into stimuli-induced reversible proton transfer, we attempted to summarize its reaction mechanism and design principle, and discuss strategies to design and prepare various related stimuli-responsive materials and devices. This Account discusses the different systems in which a color/fluorescence change is induced by the proton transfer process under various stimuli, including electric field, water, light, heat, and stress. Relative very promising applications as well as their performance especially for energy-saving and environmentally friendly devices are then summarized, such as energy-saving bistable electrochromic devices, water-jet rewritable paper, and visible-light-responsive rewritable paper. Meanwhile, we focus on the key influence factors and useful additives for improving the device's performance. At last, challenges and bottlenecks faced by stimuli-responsive materials and devices based on the mechanism of reversible proton transfer are proposed. Moreover, we put forward some suggestions on solving these limitations.These exciting results reveal that smart materials based on the mechanism of proton transfer are extremely attractive and possess great potential in the next generation of energy and resource saving and environmental protection display. We hope that this Account further prospers the field of intelligent stimuli-responsive discoloration materials and next-generation green displays.