In this contribution, lipid monolayer membrane functionalized graphene sheets were prepared using a facile method. Interactions between the graphene and different types of liposomes, including charged and neutral, were also investigated. We found that the anionic liposomes could spontaneously self-organize into lipid monolayer membranes, partially covering the surface of graphene sheets. The resultant lipid monolayer functionalized graphene nanomaterials exhibited high stability in aqueous solution and an excellent performance as carrier for loading the anticancer drug, doxorubicin (DOX), with a high loading capacity of 70%. The loaded drug can be released under pH control. 10% and 14% of the bound DOX was released after 54 h at pH 10.0 and 7.0, respectively. Whereas, about 70% of DOX was released after 54 h at pH 5.0.