Sol–gel transition accelerated by the co-assembly of two components in supramolecular hydrogels

N-Palmitoyl-Gly-His (PalGH) and glycerol 1-monopalmitate (GMP) in water co-assembled into fibrils with twisted ribbon structures and formed a homogeneous network, resulting in gel formation. Shaking the gel easily broke the fibril network leading to a sol in which high and low fibril density regions exist. After a period at room temperature, the higher density regions became interconnected. The spontaneous sol–gel transition did not take place for a gel made from only PalGH. Also, during the transition, the aggregation state of the co-assembly remained unchanged at a molecular level, unlike the fibril network. Thus, it can be claimed that the sol–gel transition is not associated with the assembled molecular configuration, but with the change in the fibril network. This knowledge might be useful for understanding and controlling sol–gel transition, thereby leading to the design and functionalization of hydrogels.