This work aims at assessing the influence of two different solvents, bidistilled water and toluene, on dispersions of carbon-based engineered nanomaterials, namely, fullerenes, and their self-assembly behavior. The obtained self-assembled carbon-based materials were characterized using UV-vis spectrophotometry and transmission electron microscopy techniques. The results obtained were unexpected when toluene was used for dispersing fullerene C60, with the formation of two different types of self-assembled structures: fullerene C60 nanowhiskers (FNWs) and a type of quasispherical nanostructure. The FNWs ranged between 1 and 6 μm in length, whereas the quasispherical fullerene C60 nanoaggregates ranged between 10 and 50 nm in diameter. Aggregates obtained in toluene showed a well-formed crystal structure. When using water, the obtained aggregates were amorphous and showed a no well-defined shape. Their sizes ranged between 20 and 40 nm for nanosized structures and between 0.4 and 4.8 μm for micron-sized self-aggregates.