The mechanism of formation and the stability of spontaneously formed vesicles upon self-assembly of a partially ground-state charge-separated, nonpolar-polar-nonpolar fullerene(C-60)-didodecyloxybenzene (DDB) dyad in binary solvent mixtures requiring a critical dielectric constant of similar to 30 are reported. Molecular interactions giving rise to defined vesicles with in-plane bilayer packing are detailed from the predominant van der Waals and electrostatic interactions existing on the dyad's framework. The vesicles are formed with a large bending rigidity of 18k(B)T, which on further extraction into a polar water medium resulted in uniform spheres that corroborated well with the theoretical predictions. Furthermore, the water-extracted spherical dyad aggregates at an increased dyad concentration, leading to the formation of giant micrometer-sized fractals following diffusion-limited cluster aggregation. These dyad aggregates act as efficient quenchers of fluorescent dyes with a quenching rate of 4.6 x 10(13) M-1 s(-1).