innovative insight into understanding the properties of the material systems beyond molecular level. [6-8] Through the last decades, supramolecular chemistry has deeply permeated and fused with biology and materials science, and has gradually growth into an interdisciplinary platform for the creation of self-assembled systems with extraordinary properties. [9-12] Among the numerous systems, self-assembled peptide is one of the most important branches, because of its rich chemical diversity, versatile characters, inherent biocompatibility, and bioactivity. [13-15] Specifically, the natural or chemically engineered amino acids encoded in the sequence of peptide molecules enable the formation of customizable secondary structures, the cooperative interactions between main chains and side chains of peptide molecules can be further leveraged to produce hierarchical nanostructures [16-22] and important biofunctions, such as drug delivery, [23-25] tissue engineering, [26-28] regenerative medicine, [29-31] and biomineralization. [32-35] Moreover, many studies have disclosed that self-assembled peptide nanostructures can offer higher performance (catalytic, therapeutic, targeting, etc.) than peptide itself. [36-42] For those reasons, peptide self-assembly has been recognized as a subject of great importance in supramolecular chemistry, biology, and nanotechnology, and the breadth and depth of peptide selfassemblies have been documented and demonstrated in several excellent reviews. [43-51] Besides the self-assembly of unimolecular peptides, multicomponent coassembly between peptides and other building blocks has recently become increasingly prevalent, as the modular approach offers a simple and effective way to arrive at supramolecular materials with wide structural complexity and value-added properties for multiple tasks applications. [52-56] This integrated characteristic further stimulates researchers to explore the scope of peptide coassembly with the aim of expanding the space of functional utility. To selectively form the multicomponent nanostructures, the interplay of the driving forces should be energetically much more favorable for strengthening the coassembly of distinct components than the self-sorting of the same type of components. [57-59] Following this design criteria, the introduction of complementary noncovalent interactions into the multicomponent systems is Peptide assembly has been extensively exploited as a promising platform for the creation of hierarchical nanostructures and tailor-made bioactive materials. Ionic coassembly of cationic peptides and anionic species is paving the way to provide particularly important contribution to this topic. In this review, the recent progress of ionic coassembly soft materials derived from the electrostatic coupling between cationic peptides and anionic species in aqueous solution is systematically summarized. The presentation of this review starts from a brief background on the general importance and advantages of peptide-based ionic coassembly. After that, divers...