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Luminescent materials with dynamic responsiveness to external stimuli have attracted extensive attention for the development of advanced sensors and smart materials; however, self-healing capability is also of great importance for functional soft materials. An acid/base vapor reversibly triggered luminescence switch with self-healing ability is achieved by incorporating dynamic lanthanide metal–ligand (Ln–L) coordination into the soft polydimethylsiloxane polymer network. The emission color of the resultant luminescent material could be modulated by altering either the Eu3+/Tb3+molar ratio or the excitation wavelength. The luminescence “On–Off” reversible switch is realized via direct alternating exposure to acid and base vapor, realizing reversible information encryption and decryption. The dynamic Ln–L cross-link as well as the hydrogen bond in the luminescent material endow it with excellent self-healing capability, high toughness, and stretchability. We believe this acid/base vapor-triggered self-healing switching strategy provides new insights for expanding the application range of luminescent materials.