An organic‐inorganic hybrid (5) is synthesized where two Dawson polyoxometalate (POM) moieties are linked to one fullerene C60 unit. In a POM‐friendly solvent such as DMSO, DMF and CH3CN, 5 forms small vesicles below 100 nm at a concentration of 37.3 mg mL–1. When the concentration decreases to 9.0 mg mL–1, detection of aggregates becomes difficult. However, supramolecular structures with diverse morphologies can be induced upon the addition of H2O or toluene. In DMSO/H2O and DMF/H2O systems, plates form, which break to debris and small vesicles at high volume percentage of H2O. In CH3CN/H2O mixtures, solid spheres form, which fail to further evolve into other self‐assembled structures. In DMSO‐based binary mixtures, the type of poor solvent has a big influence on the aggregation behavior of 5, and replacing H2O with toluene transfers the aggregates from plates to multilamellar and multicellular vesicles. In contrast, in CH3CN‐based systems, the influence of the type of poor solvent is quite limited. Although the morphologies of the aggregates change a lot, their magnetic properties remain unchanged as confirmed by electron spin‐resonance measurements.