Graphene-based nanomaterials can mediate environmentally relevant abiotic redox reactions of chlorinated aliphatic hydrocarbons. In this study as low amounts as ∼0.007 % of graphene oxide (GO) was found to catalyze the reduction of carbon tetrachloride by layered Fe(II)-Fe(III) hydroxide (Green Rust, GR) in aqueous solutions with chloroform being the reduction product. On the basis of sorption studies of carbon tetrachloride onto the GO surface it is suggested that it is the amphiphilicity of GO, which initiates the reaction by providing a suitable reaction platform for the reagents. This study indicates that traces of graphene oxide can affect reaction pathways as well as kinetics for dechlorination processes in anoxic sediments by facilitating a partial dechlorination.