Scientists have discovered a chiral compound, which can spontaneously form a molecular assembly with an extremely large single domain structure beyond a size regime incapable of realizing with usual molecular self-assembly. The chiral compound, when heated and left to cool on a solid substrate, gives a droplet featuring a single-crystal-like structure. When the substrate is set up vertically, the droplet exhibits sliding and rotating motion controlled by the chirality while preserving the single-crystalline structural order.