Metallohydrogels are attractive biomaterials, whereas formation of a selective bimetallogel in aqueous solution has rarely been explored. In this study, we show that a phenylalanine derivative containing a 4-pyridine group can not only assemble to form single crystals with copper acetate, but also selectively generate a Cu-Ag bimetallohydrogel upon further addition of silver nitrate, which exhibits excellent multi-responsiveness. This study represents a novel example of a selective bimetallohydrogel in aqueous solution, which provides insights into the formation of a bimetallohydrogel and clue...