Unprecedented self-assembled architectures of surface-active ionic liquids in aqueous medium.

The formation of ultra-thin 2D crystalline nano-sheets, -spindles and -ribbons by self-assembly of benzimidazolium-based single-tailed surface active ionic liquids (SAILs) is observed for the first time. The nature of formed bilayer architectures is governed by the functionalization of alkyl chains of SAILs via an amide or ester moiety.