A facile and scalable preparation of aqueous solutions of isolated, sparingly sulfonated graphene is reported. 13 C NMR and FTIR spectra indicate that the bulk of the oxygen-containing functional groups was removed from graphene oxide. The electrical conductivity of thin evaporated films of graphene (1250 S/m) relative to similarly prepared graphite (6120 S/m) implies that an extended conjugated sp 2 network is restored in the water soluble graphene.Recently characterized as "the thinnest material in our universe", 1 graphene, a single-atom-thick sheet of hexagonally arrayed sp 2 -bonded carbon atoms, promises a diverse range of applications from composite materials to quantum dots. [2][3][4][5][6][7] However, just as with other newly discovered allotropes of carbon (fullerenes and single-wall nanotubes), material availability and processability will be the ratelimiting steps in the evaluation of putative applications of graphene. For graphene, that availability is encumbered by having to surmount the high cohesive van der Waals energy (5.9 kJ mol -1 carbon) 8 adhering graphitic sheets to one another. Herein, we describe a facile and scalable preparation of aqueous solutions of isolated, sparingly sulfonated graphene sheets starting from oxidized graphite. The measured electrical conductivity of contiguous films of graphene prepared by evaporation of an aqueous solution implies that the extensive conjugated sp 2 carbon network is restored in the water soluble graphene.Graphene was initially isolated by mechanical exfoliation, peeling off the top surface of small mesas of pyrolytic graphite, 2,5 a method which is not suitable for large-scale application. More recently, single sheets of graphene oxide were chemically reduced to graphene after deposition on a silicon substrate, 9,10 again a method that lends itself to limited applications. Exfoliation of graphite oxidized with strong acids either by rapid thermal expansion 11 or by ultrasonic dispersion 12,13 is one approach to obtain (functionalized) graphene oxide in bulk. The oxidation chemistry is similar to that used to functionalize single-wall carbon nanotubes (SWNTs) [14][15][16] and yields a variety of oxygen functionalities (sOH, sOs, and sCOOH) primarily at "defect" sites on SWNT ends. For sufficiently strong oxidizing agents, functionalized defects were also created on the SWNT wall surfaces. 17 Therefore, independent of the exfoliation mechanics, graphene oxide prepared from oxidized graphite includes significant oxygen functionality 11 and defects so the associated structural and electronic perturbations caused by oxidation must be repaired to recover the unique properties of graphene. These perturbations can be superficially ameliorated with "passivation chemistry," for example, reacting graphene oxide with amines, 12 but the resulting materials are not expected to exhibit the electronic attributes of graphene because of residual (passivated) defects.Ideally graphene oxide must be rigorously reduced after exfoliation to recover the desirable ...