Structural and morphological regulation is a distinctly important topic in peptide self-assembly, and is also regarded as the fundamental point in peptide-based biomaterials development. In this paper, we showed that adding anionic surfactant SDS to a bola amphiphilic peptide KI4K could result in the reconstruction of β-sheet secondary structure besides the changes in self-assembly morphologies from nanotubes to helical ribbons, nanofibers, or straight nanotapes according to the negatively stained transmission electron microscopy, atomic force microscopy, circular dichroism spectroscopy, and Fourier transform infrared spectroscopy results. The inducing effect of SDS was observed at both above and below its CMC but with different transformation rates. Through comparison to other surfactants, including CTAB, C12EO4, and AOT, we proposed that the transitions of KI4K self-assemblies induced by anionic surfactants could be mainly attributed to the effect of hydrophobic interaction and electrostatic attraction between surfactants and peptide molecules. Rheological property measurement and dye adsorption experiments were also carried out to evaluate the properties of hydrogels formed by the peptide/surfactant hybrids. The samples formed self-supporting hydrogels at proper SDS or AOT concentrations, and the charges of hydrogel could be regulated by peptide to surfactant ratio.