Carbon microspheres (CMS) with size of 370 nm were synthesized by chemical vapor deposition. Then CMSs were oxidized with a mixture of concentrated HNO3 and H2O2 Finally, CMSs were covered with ZnO to form ZnO/CMS composites after CMSs were reacted with zinc acetate and triethanolamine. The influences of molar ratio of zinc acetate to triethanolamine and reaction time were investigated. The morphology and structure of the products were characterized by field emission scanning electron microscopy, Fourier transformation infrared spectrometry, thermogravimetry and Xray diffraction. The results show that the obtained ZnO/CMS composites with uniform size had smooth surfaces and the interaction between ZnO and CMSs was stronger when the molar ratio of zinc acetate to triethanolamine was 1 2 and the reaction time was 2 h.