Radioactive Cs is a major by-product of nuclear power plants, with high radioactivity and long half-life. It is highly soluble in water and is difficult to remove. In this study, pristine graphene oxide (GO) synthesized via a Hummer's method has been demonstrated as a very efficient Cs sorbent with the maximum adsorption capacity of GO found to be 180, 465, 528 mg Cs/g sorbent at pH of 3, 7, and 12, respectively. The results from Fourier-transform infrared (FTIR) spectroscopy of GO before and after Cs sorption at various pH values reveal the mechanism of Cs sorption by GO. Several functional groups which are carboxyls, phenols, and hole defects containing multi-ether groups, are shown to play an important role in Cs capture. GO's affinity for other major cations found in seawater, namely, Na, K, and Mg was also evaluated, and the effect of these cations in competing with Cs for adsorption on GO was also studied. This reveals GO's exceptional ability in capturing Cs even in the presence of high concentrations of competitive cations and its high potential for use in Cs decontamination, as well as other heavy metal removal applications.