Washboard belt-like zinc selenide (ZnSe) nanostructures are successfully prepared by a simple chemical vapor deposition (CVD) technology without catalyst. The phase compositions, morphologies and optical properties of the nanostructures are investigated by X-ray diffraction (XRD), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM) and photoluminescence (PL) spectroscop, respectively. A vapor-liquid mechanism is proposed for the formation of ZnSe belt-like structures. Strong PL from the ZnSe nanostructure can be tuned from 462 nm to 440 nm with temperature varying from 1000 °C to 1200 °C, and it is demonstrated that the washboard belt-like ZnSe nanostructures have potential applications in optical and sensory nanotechnology. This method is expected to be applied to the synthesis of other II-VI groups or other group’s semiconducting materials.