Graphene oxide can strongly affect the fate of chlorinated solvents under anoxic iron-rich conditions. Trace amounts of graphene oxide was found to strongly facilitate the reduction of carbon tetrachloride by green rust. Chloroform was the sole and “dead end” dechlorination product. The amphiphilicity of GO is responsible for the enhanced dechlorination. GO can provide a suitable reaction platform for carbon tetrachloride by green rust.