Zinc oxide is one of the most important wide-band-gap (3.2 eV) materials with versatile properties, however, it can not be excited by visible light. In this work, we have developed an exquisite and simple way to prepare oxygen-deficient ZnO 1-x nanosheets with a gray-colored appearance and excellent visible light photocatalytic activity. Detailed analysis based on UV-Vis absorption spectra, X-band electron paramagnetic resonance (EPR) spectra, and photoluminescence (PL) spectra confirms the existence of oxygen vacancies in ZnO 1-x. The incorporation of oxygen defects could effectively extend the light absorption of ZnO 1-x into the visible-light region due to the fact that the energy of the localized state is located in the forbidden gap. Thus, our obtained ZnO 1-x shows a higher photodegradation of methyl orange (MO) compared to defect-free ZnO under visible light illumination. Additionally, the high content of ˙OH radicals with a strong photo-oxidation capability over the ZnO 1-x nanosheets significantly contributes to the improvement in the photocatalytic performance. Our oxygen deficient ZnO 1-x sample shows a very high photocatalytic activity for the degradation of MO even after 5 cycles without any obvious decline. The results demonstrate that defect engineering is a powerful tool to enhance the optoelectronic and photocatalytic performances of nanomaterials.