Surfactants are widely used for dispersing graphene and functionalized graphene sheets (FGS) in colloidal suspensions, but there have been few studies of the structure of the dispersed graphene–surfactant complexes in suspension and of their time evolution. Here, we combine experimental study of efficiencies of ionic surfactants/polymers in suspending FGS in water with characterization using atomic force microscopy, small angle neutron scattering, and molecular simulations to probe the detailed structures of FGSs. The small angle scattering technique provides quantitative measurement of structure of graphene sheets in the solution. This study suggests that in both ionic and nonionic surfactants, the dispersion tends to degrade over time through detachment of the surfactant molecules and structural rearrangements. Ionic surfactants with strong interfacial binding and large molecular weight increase the dispersing power by over an order of magnitude.