Graphene aerogel was synthesized and used for the removal of methyl blue from aqueous solutions. The effect of solution pH, temperature and adsorption time on the adsorption performance of the graphene aerogel was studied systematically. In addition, investigations were also performed to determine the nature of adsorption. The experimental results show that graphene aerogel is a highly efficient adsorbent for the treatment of methyl blue in aqueous solutions. In addition, the adsorption of methyl blue proceeds through a single layer physical adsorption on the graphene aerogel. The findings herein are useful for the future development of adsorbent for in water.