An amphiphilic dendron containing three dendrite L‐glutamic acid units and a long alkyl chain was synthesized by a convergent method. It was found that the dendron could form hydrogels over a wide pH range from 2 to 13. Moreover, accompanying the pH change, the compounds self‐assembled into various chiral structures: from helical nanotube, helical nanotube with a string of beads, and coiled superhelix to dendrite nanostructures, such as pine, feather, etc. A series of characterizations based on TEM observations, X‐ray diffraction and FTIR spectroscopic measurements revealed that the dendron formed a bilayer first and then hierarchically self‐assembled into various chiral nanostructures. The four carboxylic acid groups and three amide groups played an important role in the self‐assembly. The interaction between the multiamide groups stabilized the bilayer structures, whereas the ionization degree of the carboxylic acids was responsible for the formation of various chiral structures. The work presented a hydrogel system with wide pH adaptability and showed the regulation on chiral structures by simple pH variations.