Versatile Grafting Approaches to Functionalizing Individually Dispersed Graphene Nanosheets Using RAFT Polymerization and

*S Supporting Information ABSTRACT: Developing powerful and reliable strategies to covalently function-alize graphene for efficient grafting and achieving precise interface control remains challenging due to the strong interlayer cohesive energy and the surface inertia of graphene. Here, we present versatile and efficient grafting strategies to functionalize graphene nanosheets. An alkyne-bearing graphene core was used to prepare polymer-functionalized graphene using ‘grafting to ’ and ‘grafting from’ strategies in combination with reversible chain transfer and click chemistry. The use of the ‘grafting to ’ approach allows full control over limited length grafted polymer chains, while permitting a high grafting density to a single graphene face, resulting in good solubility and processability. The ‘grafting from ’ approach offers complementary advantages, such as the grafting of high molecular weight polymer chains and a better coverage ratio on the graphene surface; however, the extra steps introduced, the presence of initiating groups, and difficulty in controlling the grafted polymer lead to decreased processability. Various types of polymer chains have been successful covalently tethered to graphene nanosheets using these two approaches, producing various molecular brushes with multifunctional arms resulting in water-soluble, oil-soluble, acidic, basic, polar, apolar, and variously functionalized polymers. This work describes versatile methodologies, using the ‘grafting to ’ and ‘grafting from ’ approaches, for the preparation of individually dispersed graphene nanosheets having the desirable properties described