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• All dispersants considered acted in synergy with resins in peptizing asphaltenes. • Ionic liquid yielded the best dispersing power and the highest self-association. • Significant electron-withdrawing sites were main contributors to dispersing power. • Steric hinderance associated with molecular structure affected dispersing behavior. In confronting the global climate change, reusing waste asphalt materials stands out as a key strategy for the transportation sector to preserve natural resources and reduce the carbon footprint. Recycling additives or rejuvenators are usually required in this practice, especially for boosting the recycling rate. Given the imperative need for a general compositional design principle of rejuvenators, we previously proposed an innovative formulation concept by combining softeners with asphaltene dispersants, and reported that the use of dispersants largely reduced the total quantity of rejuvenators needed and thus would minimize the environmental impacts. The present study is aimed for probing the molecular mechanisms underlying this observation, with additional interest focused on the synergistic effect of the dispersants with resins and also on the impacts due to their self-association. Selection of representative materials consisted of three types of dispersants including an ionic liquid, a phenolic amphiphile, and an ester plasticizer, in combination with an aromatic oil as the softener. Long-time molecular dynamics (MD) simulation was employed to inspect the aggregation of asphaltenes. Quantum chemical (QC) computation was performed to provide insights into the source of different dispersing behaviors. The results indicated that the three dispersants all acted in concert with resins in dispersing asphaltenes. The dispersion characteristics of asphaltenes could be viewed as a net result of the two competing mechanisms of the dispersing capability and self-association of the dispersant used. The ionic liquid exhibited much higher propensity to self-association at increasing concentrations than the phenolic dispersant, and yet the optimum performance was achieved for both when they were added at low dosages. The ester plasticizer showed minimal self-association and yielded improved dispersion with increasing concentrations. In all cases, the dispersing functionality mainly originated from the presence or formation of significant electron-withdrawing sites, collectively due to the highly electronegative cation and anion, hydrogen bonding, and polar groups. Comparison of the dispersing power was also conducted from different perspectives. The findings are expected to provide molecular insights for formulating versatile and more environmentally benign asphalt rejuvenators. [ABSTRACT FROM AUTHOR]