Zinc oxide (ZnO) has been widely used as a photocatalyst for solar energy conversion and treatment of organic pollutants because of its low toxicity and high photocatalytic efficiency. However, the applicability of ZnO in visible light is limited because of the wide band gap of the material, which results in low efficiency during solar photoconversion. In this paper, we report the facile one-pot, morphology-controlled, and large-scale synthesis of carbon-doped ZnO through urea-assisted thermal decomposition of zinc acetate. Nanorods and nanospheres of carbon-doped ZnO were successfully prepared by using this one-step method with various weight percent of urea. The photocatalytic activities of nanocrystals obtained with different morphologies and carbon contents were evaluated through degradation of methylene blue with visible light irradiation. Results showed that incorporation of carbon decreases the energy band gap of ZnO, improves the separation efficiency of its electron-hole pairs, and significantly enhances the visible light photocatalytic activity.