Zinc oxide (ZnO) nanostructures were synthesized via a one‐step solid‐state reaction approach in ammonia (NH3) gas environment with different temperature ramp rates. The so‐formed nanostructures were characterized using X‐ray diffraction (XRD) for phase identification, where the typical wurtzite hexagonal structure was observed. Scanning electron microscopy (SEM) confirmed the particle size to be in the range 45–50 nm, the same as calculated by the XRD pattern for the ramp rate of 10 °C/min. Energy dispersive X‐ray (EDX) spectroscopy and X‐ray photoelectron spectroscopy (XPS) confirmed the chemical purity of the samples. The photoluminescence (PL) spectrum indicated multiple near‐band‐edge emissions and energy‐band emissions. Then, these ZnO nanomaterials were used for the degradation of crystal violet (CV) dye under UV light irradiation. The CV solution was completely degraded in 2 hr. The initial photocatalyst and dye amounts of 0.2 g/100 ml and 0.5 mg/L, respectively, were found to be the optimum values for maximum degradation efficiency. The ZnO‐based photocatalyst was stable up to three cycles of reuse. These results indicate that the high surface area and porosity of the nanomaterials are responsible for the high efficiency, which was confirmed by specific surface area analysis.