In this study, oxygenated graphene nanosheets (OGNs) were successfully synthesized using a simple electrochemical exfoliation approach and applied to remove methylene blue (MB) in an aqueous solution. The surface morphology and structure of the OGNs were characterized by scanning electron microscopy, transmission electron microscopy, Raman, and x-ray photoelectron spectroscopy. The adsorption performance of OGNs towards aqueous MB was tested by batch experiments. Results showed that a large number of functional groups in OGNs enhanced the removal of MB from the aqueous solution due to the electrostatic interactions between the electrochemically oxygenated groups (e.g. C-OH, C-O, and C=O) and dye molecules. Using Langmuir adsorption isotherm, the maximum MB adsorption capacity (q max) was determined as high as 476.19 mg g-1. These results suggested that the as-prepared OGNs is an effective and promising adsorbent for removing MB, which could be studied extensively for color removal in wastewater treatment.