A clear correlation between defect-related emissions and the magnetization of ZnO nanorods synthesized by a one-step aqueous chemical method is demonstrated. The relative contribution of the emission bands arising from various types of defects is determined and found to be linked with the size of the nanorods and annealing conditions. When the size of the nanorods and the annealing temperature are increased, the magnetization of pure ZnO nanorods decreases with the reduction of a defect-related band originating from singly charged oxygen vacancies (). With a sufficient increase of annealing temperature (at 900 °C), the nanorods show diamagnetic behavior. Combining with the electron paramagnetic resonance results, a direct link between the magnetization and the relative occupancy of the singly charged oxygen vacancies present on the surface of ZnO nanorods is established.