We report herein the self-organization of the polymerizable bolaamphiphile (noted, L-Asp-DA) that contains a diacetylene group and two L-aspartic groups. We found that L-Asp-DA can self-organize into stable fiberlike nanostructures at the mica-water interface. The micellar nanostructures of L-Asp-DA can be polymerized both ill the bulk solution and in the Film on UV irradiation, and the nanostructures of the L-Asp-DA micelles at the mica-water interface can be maintained after polymerization. The polymerized L-Asp-DA nanostructures can go through blue-red transition upon pH stimuli arising from the transformation of polydiacetylene skeleton. Ill addition, the concentration (above cmc) of L-Asp-DA has a great effect on the nanostructures. At a concentration of 3.2 x 10(-4) mol/L, L-Asp-DA can self-organize into stable fiberlike nanostructure at the mica-water interface, while cylindrical nanostructures self-organize at a concentration of 6.0 x 10(-4) mol/L. This work may provide a new approach for designing and fabricating molecular assemblies with controlled sizes and shapes, leading to the development of novel functional polymer nanostructure materials.