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The results of experiments on the self-aggregation of C60 fullerene molecules both inside a two-component solvent (xylene/tetrahydrofuran) and in the volume of an evaporating drop of C60 colloidal solution on a flat substrate surface are presented. The investigations of C60 solutions using dynamic light scattering, transmission electron microscopy and UV–Vis absorption spectroscopy methods revealed the possibility of synthesis of fractal nanoaggregates with a diameter of up to ~135 nm at low concentrations of C60 in the solutions. The final geometric dimensions of C60 nanoaggregates were determined by the initial concentration of fullerene in the solvent medium. Using the scanning electron microscopy method, we have shown that in an open dissipative system – in the volume of an evaporating droplet of the colloidal solution of fullerene C60 sessile on the surface of a flat glass substrate, large quasispherical nanoaggregates with an average diameter of ~380–800 nm are formed. The physical features and regularities that characterize the processes of self-aggregation of fullerene particles in the volume of a drying drop were determined.