The structure of graphite oxide (GO) has been systematically studied using various tools such as SEM, TEM, XRD, Fourier transform infrared spectroscopy (FT-IR), X-ray photoemission spectroscopy (XPS), 13C solid-state NMR, and O K-edge X-ray absorption near edge structure (XANES). The TEM data reveal that GO consists of amorphous and crystalline phases. The XPS data show that some carbon atoms have sp3 orbitals and others have sp2 orbitals. The ratio of sp2 to sp3 bonded carbon atoms decreases as sample preparation times increase. The 13C solid-state NMR spectra of GO indicate the existence of - OH and - O - groups for which peaks appear at 60 and 70 ppm, respectively. FT-IR results corroborate these findings. The existence of ketone groups is also implied by FT-IR, which is verified by O K-edge XANES and 13C solid-state NMR. We propose a new model for GO based on the results; - O - , - OH, and - C = O groups are on the surface. © 2010 American Chemical Society.