In this work, an interfacial synthetic strategy to produce ZnO troughs at the air-water interface under mild conditions was demonstrated. The as-prepared ZnO trough was monodisperse, single crystalline, and pure. By manipulation of the magnet stirring time, the fabricated ZnO can be manipulated as an independent or intertwined trough. Various preparative parameters, such as initial reactants and their concentrations, had been examined, and the results revealed that troughlike ZnO could be only obtained by adopting zinc acetate and hexamethylenetetramine as precursors at concentrations larger than 0.01 M. The as-obtained ZnO, within the dimension of several micrometers, showed a trough-related photoluminescence emission at 356 nm. Moreover, the evolution process of a ZnO trough after reaction for 5, 30, 60, and 90 min was viewed by X-ray diffraction and field emission scanning electron microscopy characterization, and a possible mechanism was also proposed and discussed, which might help us to further our understanding toward the reaction mechanism at the air-water interface.