Vesicles, closed bilayer structures composed of amphiphiles, have attracted considerable attention as functional materials. Structural stability and stimulus responsiveness are required for next-generation functional vesicles. However, there is a dilemma between these properties because the desired membrane structure varies in terms of structural stability and stimulus sensitivity. Herein, we propose a new approach for the development of giant vesicles (GVs) through the molecular design and synthesis of amphiphiles with or without amide linkages, forming hydrogen bonding. From the