The layered sodium cobalt oxide Na0.6CoO2 phase has been synthesized from Na2O2 and Co3O4 by solid-state reaction at 550°C for 12h with the heating rate about 2°C /min. The colloidal suspension of exfoliated, layered cobalt oxide nanosheets was prepared through the intercalation of tetrabutyl ammonium hydroxide ions (TBA) into protonated sodium cobalt oxide. The as-obtained composites were analyzed by powder X-ray diffraction (XRD). They were also cross-confirmed by a range of methods including UV/Vis spectroscopy, and Transmission Electron Microscopy (TEM). The Zeta-potential measurements clearly demonstrated the negative surface charge of cobalt oxide nanosheets.