Understanding the molecular interactions between suspended nanoparticles (NPs) and the suspending solvent fluid may provide a useful avenue to create and to study exotic NP ensembles. This study focused on using a coarse-grained computational model to investigate the molecular interactions between oleate-capped NPs in various solvents, and to relate the results to experimental features of solvent-suspended, oleate-capped CdSe quantum dots (QDs). The QDs were modeled as a closed-shell fullerene molecule with an oleate-like ligand attached to each vertex. Solvent polarity was found to correlate to the simulation and experimental results more strongly than either dielectric constant or dipole moment. Computational results showed that the nonpolar solvents of hexane, toluene, and benzene (polarity index E-T(N) < 0.120) kept NPs in suspension and solvated the oleate chains such that the oleate layer swelled to full extension. In contrast, as the most polar solvent tested (E-T(N) = 1.000), water caused NPs to aggregate and precipitate. It partially solvated the oleate chains and compressed the layer to 86% of full extension. For solvents of intermediate polarity like ethanol, acetone, and chloroform, the oleate layer swelled with decreasing polarity index values, with rapid swelling occurring close to E-T(N) = 0.307 (similar to 50:50 vol % chloroform/acetone) below which QDs were colloidally stable. This study represents the first attempt to delineate the solvent effect on surfactant-coated NP hydrodynamic size, colloidal stability, and aggregation behavior.