Molecular dynamics (MD) simulations were used to study the nanoaggregation of model asphaltene molecules in binary mixtures of toluene and water. Four types of model asphaltenes were studied: continental (C), Violanthrone-79 (VO-79), anionic continental (AC), and thiophenic anionic continental (TAC). Of these, the first two were uncharged, whereas the AC and TAC contained a side chain with a carboxylic terminal group. In all simulations, the model asphaltenes partitioned completely into the toluene phase of the phase-separated solvent mixture. The asphaltene molecules containing charged terminal groups remained tethered to the toluene-water interface (interface-bound), whereas uncharged asphaltenes aggregated within the central region of the toluene layer (core-bound). The stacked polyaromatic rings of the asphaltene aggregates showed a distinct preference to incline almost perpendicular to the toluene-water interface. Analysis of the mean square displacements of the asphaltenes reveals that for both charged and uncharged model asphaltenes, the lateral diffusion parallel to the toluene-water interface is dominant, whereas the transverse diffusion (normal to the interface) becomes significantly suppressed. This observation suggests that in thin films',of toluene trapped between two aqueous phases, both interface-bound and core-bound asphaltenes, although subjected to vastly different interaction scenarios, exhibit similar diffusion behavior.