In the present work, a new supramolecular gel of azobenzene-based phenylalanine derivative (AZO-Phe) and its application in methylene blue (MB) adsorption have been developed. The gelator has shown great ability to form stable gels with a critical gelation concentration as low as 1.0 mg/mL in EtOH/H 2 O. The studies also showed that the gel has a good adsorptive performance to MB in aqueous solution. The adsorption process and mechanism of MB on AZO-Phe gel was systematic investigated. Batch experiments were performed to study the effects of initial dye concentration, contact time and pH on the adsorption performance of AZO-Phe gel. The adsorption process and data was fitted well with Langmuir isotherm model and pseudo-second-order kinetic model. Moreover, AZO-Phe gelator could be recovered after MB adsorption, and rate of recovery was achieved 95%. These results provide a mixed solvent gel method for the purification of dye-polluted water systems, while also paving the way for future design of functionalized supramolecular self-assemble systems.