Application of dilational surface rheology, surface tensiometry, ellipsometry, Brewster angle, and transmission electron and atomic force microscopies allowed the estimation of the structure of the adsorption layer of a fullerenol with a large number of hydroxyl groups, C60(OH) X ( X = 30 ± 2). The surface properties of fullerenol solutions proved to be similar to the properties of dispersions of solid nanoparticles and differ from those of the solutions of conventional surfactants and amphiphilic macromolecules. Although the surface activity of fullerenol is not high, it forms adsorption layers of high surface elasticity up to 170 mN/m. The layer consists of small interconnected surface aggregates with the thickness corresponding to two-three layers of fullerenol molecules. The aggregates are not adsorbed from the bulk phase but formed at the interface. The adsorption kinetics is controlled by an electrostatic adsorption barrier at the interface.