The production of graphite oxide from graphite usually requires strong oxidants, concentrated acids, and a reaction time of the order of 100 h. In this study, we adopted a highly efficient cathodic plasma (CP) process in which the vapor plasma envelope calorific effect provides instant oxidation and expansion of graphite for producing plasma-expanded graphite oxides (PEGOs) from recycled graphite electrodes (GEs) or high purity graphite (HG), within a reaction time of 10 min without the need for strong oxidants or concentrated acids. X-ray diffraction, X-ray photoelectron spectroscopy and Raman spectroscopy confirmed the dramatic structural change from GEs or HG to graphite oxides after the CP process. Furthermore, scanning electron microscopy and transmission electron microscopy revealed that the graphite oxide possessed a spheroidal morphology, with dimensions of 1-3 μm, as a result of melting and subsequent quenching during the plasma electrolysis process. We obtained a stable, homogeneous dispersion of PEGOs in N-methyl-2-pyrrolidone after sonication and filtering of the centrifuged PEGOs. We used these spheroidal graphite oxide particles as effective adsorbents for the removal of pollutants (e.g., Methylene Blue) from aqueous solutions. These PEGOs also served as good precursors for the preparation of graphite nanoplatelets. CP processing appears to be an effective and environmentally friendly means for mass-producing graphite oxide.