925wileyonlinelibrary.com COMMUNICATION performance. By analogy to the aforementioned graphene and metallic oxide composites, the hybrids of graphene and fullerenes is expected to create a new class of active materials with the strong electron-accepting capability characteristic of fullerenes and the good charge transport properties associated with graphene. Similarly, our previous study has shown that the assembly of C 60 derivatives and single-walled carbon nanotubes (SWCNTs) are promising for photovoltaics. [ 29 ] Compared with SWCNTs, which are 1D and a mixture of semiconducting and metallic, graphene is 2D and has purely semimetal characteristics, thus providing a more preferred geometry and a simpler electronic structure to collaborate with C 60 , promoting the charge separation and charge transfer.Various fabrication methods have been explored for obtaining a single layer graphene nanosheet. [ 14,30 ] Among them, along with the breakthrough isolation of a single layer of graphene from a graphite surface by the adhesive tape method, [ 31 ] chemical treatment of solution-dispersible graphene has received intense interest and is regarded as one of the most cost-effective and tractable preparation methods. [ 32,33 ] In general, graphite is converted to solution dispersible graphite oxide (GO) by oxidation-based intercalation followed by a chemical reduction which turns GO to graphene (strictly referred to as reduced graphene oxide, rGO). Most oxygen-containing substituent groups can be removed by chemical reduction; however, a large number of defects remain in the rGO, which leads to considerable disruption of the favorable electronic properties of graphene. [ 32,34 ] Great efforts have been devoted to directly exfoliating graphite into graphene sheets, i.e., exfoliating graphite by sonicating it directly in organic solvents [ 35 ] or with the aid of organic intercalators/surfactants. [36][37][38] However, the amount of exfoliated graphene is usually very little relative to the starting material and the actual yield is typically less than 1%. Moreover, the resulting graphene tends to agglomerate or restack through van der Waals interactions. In this regard, there is a highly important demand to develop a methodology of producing large quantities of unoxidized graphene containing fewer defects and simultaneous compositing with other functional molecules for improving their optoelectronic properties.Here, we show that graphene of high quantity is directly exfoliated from graphite in organic solvents in the presence of an alkylated-C 60 molecule ( 1 , Figure 1 a), which is 3,4,5-tris(eicosyloxy)phenyl substituted N -methyl[60]fulleropyrrolidine, [ 39 ] through noncovalent attractive interactions. Importantly, for the as-obtained 1-graphene assembly, graphene boosts nearly 270-fold higher photocurrent than 1 itself.As we reported recently, SWCNTs are mostly unbundled due to the assembly with 1 and well-dispersed in organic solvents,