Double-stranded helical crystals with high axial ratio are prepared from a cholic acid ester. Two processes are involved in the formation of the micrometer-scale self-assembled crystals: 1) the self-assembly of the cholic acid ester to form a hydrogel (the formation of gel fibers); 2) the winding of the gel fibers (laser confocal scanning micrographs show, top: left-handed; bottom: right-handed).