A concentrated nitric acid solution was used as an oxidant to modify the electrochemical performance of natural graphite as anode material for lithium ion batteries. Results of X-ray photoelectron spectroscopy, electron paramagnetic resonance, thermogravimmetry, differential thermal analysis, high resolution electron microscopy, and measurement of the reversible capacity suggest that the surface structure of natural graphite was changed, a fresh dense layer of oxides was formed. Some structural imperfections were removed, and the stability of the graphite structure increased. These changes impede decomposition of electrolyte solvent molecules, co-intercalation of solvated lithium ions and movement of graphene planes along the a-axis direction. Concomitantly, more micropores were introduced, and thus, lithium intercalation and deintercalation were favored and more sites were provided for lithium storage. Consequently, the reversible capacity and the cycling behavior of the modified natural graphite were much improved by the oxidation. Obviously, the liquid–solid oxidation is advantageous in controlling the uniformity of the products.