Zwitterions are organic salts whose cation and anion are covalently bridged. In the Focus Review, I describe the potential utility of these zwitterions as building blocks for self-organizing materials, such as liquid crystals and block copolymers. Owing to the unique characteristics of zwitterions to form homogeneous mixtures with certain acids and lithium salts, their self-organization behavior can be tuned by addition of these compounds. In particular, these zwitterion derivatives are useful for constructing bicontinuous cubic liquid-crystalline assemblies with three-dimensionally continuous periodic minimal surface.