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Abstract: Utilizing supramolecular assembling system to achieve tunable photoluminescence emission has become an important method for the development of light‐emitting materials, which could bring out intriguing photophysical properties out of the luminophores themselves without a demanding design and tedious chemical synthesis. In the last few years, vibration‐induced emission (VIE) molecules, with dual photoluminescence emissions and large Stokes shift, have shown their talent in generating tunable fluorescence and potential in fabricating novel light‐emitting materials. However, little attention has been devoted to explore the attractive properties of VIE molecules in supramolecular self‐assembling systems up to now. Herein, the first example of a supramolecular assembling system composed of a water‐soluble VIE molecule N,N′‐diphenyl‐dihydrodibenzo[a,c]phenazines derivative (DPAC‐AB) and bis‐p‐sulfonatocalix[4]arene (BSC4) is introduced. Based on noncovalent interactions including hydrophobic interaction and host–guest interaction between DPAC‐AB and BSC4, tunable fluorescence emissions from orange‐red to white (Commission Internationale de L'éclairage (CIE) coordinates (0.32, 0.37)) to blue are achieved by simple addition of different amounts of BSC4 to the solution of DPAC‐AB. Additionally, a competitive guest acetylcholine is utilized to recover the nearly orange‐red fluorescence emission. This strategy to efficiently control the emission of VIE molecules through supramolecular assembling based on reversible noncovalent interactions opens new avenues in developing tunable light‐emitting materials. [ABSTRACT FROM AUTHOR]