Biomimetic and bioinspired materials are receiving increasing attention because of their robust functionality and potential applications as artifi cial tissue [1,2]. For natural materials, a high degree of sophistication is achieved through self-organization of the various components into ordered and hierarchical structures following a well-defi ned pattern [2][3][4]. Biological tissue possesses these ordered structures, endowing the living organisms with mechanical toughness and functionality, as exemplifi ed by tissues such as bone and cartilage. Th erefore, eff orts should be made to introduce ordered and hierarchical structure into soft, and also hard, synthetic materials. Among the strategies developed to date, self-assembly is a convenient and powerful method for producing ordered structures [5].Self-assembly, the spontaneous organization of discrete components into organized structures, is widespread in nature, such as in protein folding and hybridization of the DNA double helix [3][4][5][6]. Self-assembled structures usually incorporate additional functionalities. For example, phospholipids form a lipid bilayer arou nd the cell as a barrier to the diffusion of ions and proteins, and tropocollagens self-assemble into fi brils collagens that are closely packed in parallel arrays in the tendon, endowing it with excellent mechanical properties [3]. Inspired by nature, molecular self-assembly that is directed through weak, noncovalent interactions has received tremendous attention for the development of systems with ordered structures and resultant functions [1,2,6,7]. Th ese eff orts have resulted in various functional materials based on self-assembled structures including solutions, elastomers, gels and hard materials [1,2,[7][8][9].Gels as a functional system is an emerging fi eld in themselves, possessing a responsiveness to external stimuli such as stress, light, temperature, pH and ionic strength [10]. Gels with molecular assemblies can be produced in organic solvent (organogels) or aqueous solvent (hydrogels). In this review, we focus primarily on functional hydrogels with self-assembled structures. Functional organogels produced by molecular self-assembly have been covered in several excellent reviews [11][12][13][14].Hydrogels as a functional material have their own advantages over organogels. Th e aqueous medium makes hydrogels an ideal candidate for soft biotissue, mimicking its functions for applications such as scaff olds for cell culturing [15,16]. However, producing structured hydrogels is not easy because the ordered structure formation and water content (which introduces fl uctuation) work in opposite directions. Th e typical kinds of molecules capable of forming self-assembled structures in aqueous media are amphiphile, block-copolymer and liquid-crystalline (LC) molecules. Under certain conditions, the ordered structures formed by molecular self-assembly can be frozen in physically or chemically crosslinked hydrogels with additional functionalities, such as anisotropic optical and mechanica...