The flowerlike ZnO nanostructures, which consisted of swordlike ZnO nanorods, have been prepared by a cetyltrimethylammonium bromide (CTAB)-assisted hydrothermal process at low temperature (120 °C). The XRD pattern indicated that the flowerlike ZnO nanostructures were hexagonal. Furthermore, the SAED and HRTEM revealed that the swordlike ZnO nanorods were single crystal in nature and preferentially grew up along [001]. Finally, the mechanism for the CTAB-assisted hydrothermal synthesis of flowerlike ZnO nanostructures has been preliminarily explained by polar crystal growth theory and surfactant action theory.