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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 in 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. In addition, the concentration (above cmc) of l-Asp-DA has a great effect on the nanostructures. At a concentration of 3.2 × 10−4mol/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 × 10−4mol/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. [ABSTRACT FROM AUTHOR]