Supramolecular [60]Fullerene Liquid Crystals Formed By Self-Organized Two-Dimensional Crystals

Fullerene‐based liquid crystalline materials have both the excellent optical and electrical properties of fullerene and the self‐organization and external‐field‐responsive properties of liquid crystals (LCs). Herein, we demonstrate a new family of thermotropic [60]fullerene supramolecular LCs with hierarchical structures. The [60]fullerene dyads undergo self‐organization driven by π–π interactions to form triple‐layer two‐dimensional (2D) fullerene crystals sandwiched between layers of alkyl chains. The lamellar packing of 2D crystals gives rise to the formation of supramolecular LCs. This design strategy should be applicable to other molecules and lead to an enlarged family of 2D crystals and supramolecular liquid crystals. Soft materials: A series of fullerene dyads self‐organize to form two‐dimensional crystals through π–π interactions between fullerenes. Lamellar packing of the 2D crystals gives rise to the formation of a new family of thermotropic supramolecular liquid crystals with hierarchical structures.