Peptide amphiphiles (PAs) are extremely attractive as molecular building blocks, especially in the bottom-up fabrication of supramolecular soft materials, and have potential in many important applications across various fields of science and technology. In recent years, we have designed and synthesized a large group of peptide amphiphiles. This library of PAs has the ability to self-assemble into a variety of aggregates such as fibers, nanosphere, vesicles, nanosheet, nanocups, nanorings, hydrogels, and so on. The mechanism behind the formation of such a wide range of structures is intriguing. Each system has its individual method of aggregation and results in assemblies with important applications in areas including chemistry, biology, and materials science. The aim of this feature article is to bring together our recent achievements with designer PAs with respect to their self-assembly processes and applications. Emphasis is placed on rational design, mechanistic aspects of the self-assembly processes, and the applications of these PAs. We hope that this article will provide a conceptual demonstration of the different approaches taken toward the construction of these task-specific PAs.