Self-assembling surfactant-like peptides have been explored as emerging nanobiomaterials in recent years. These peptides are usually amphiphilic, typically possessing a hydrophobic moiety and a hydrophilic moiety. The structural characteristics can promote many peptide molecules to self-assemble into various nanostructures. Furthermore, properties of peptide molecules such as charge distribution and geometrical shape could also alter the formation of the self-assembling nanostructures. Based on their diverse self-assembling behaviours and nanostructures, self-assembling surfactant-like peptides exhibit great potentials in many fields, including membrane protein stabilization, drug delivery, and tissue engineering. This review mainly focuses on recent advances in studying self-assembling surfactant-like peptides, introducing their designs and the potential applications in nanobiotechnology.