Abstract: The present disclosure provides methods of forming graphene-containing microcapsules, which may include steps of providing a graphene-containing precursor, combining the graphene-containing precursor with a drying oil such that the drying oil is intercalated within the graphene-containing precursor to form a graphene-containing aggregate, adding the graphene-containing aggregate to an aqueous solution comprising an emulsifier, and adding an encapsulating agent to form graphene-containing microcapsules. The graphene-containing microcapsules of the present disclosure may be used in numerous applications including in self-healing materials.