A real rejuvenator must have the ability to disaggregate oxidized asphaltene nanoclusters. However, few studies pay attention to the topic, and there is a lack of comparison of the disaggregation ability of different rejuvenators. Thus, the disaggregation ability and regeneration mechanism of three bio-rejuvenators (waste cooking oil (WCO), waste wood oil (WWO), and straw liquefied residue oil (SLRO)) on oxidized asphaltene nanoclusters were studied in this paper. Laboratory tests and molecular dynamics (MD) simulation were used to compare the effectiveness of the three bio-rejuvenators and reveal its corresponding mechanism. It is found that these bio-rejuvenators have a softening effect on aged asphalt binder, but not all of them can disaggregate oxidized asphaltene nanoclusters. The introduction of WWO and WCO can effectively disturb the nanoclusters caused by the increase of polar functional groups during the oxidation process. The effect of WWO is more significant, but neither of them can restore the asphaltene dispersion to the virgin asphalt binder. SLRO has an adverse effect on the disaggregation of oxidized asphaltene nanoclusters. WCO, WWO, and SLRO showed different disaggregation mechanisms, including ″pull-out, intercalation, and compression″, respectively. WCO and WWO can increase the activation energy reduced by aging in a short aging time, and SLRO makes the activation energy lower. Such findings can help enterprises screen more reasonable rejuvenators to facilitate the recycling of reclaimed asphalt pavement (RAP) materials and promote the sustainable development of the construction industry.

In order to study the characteristics and laws of nanocrack generation and self-healing behavior of asphalt materials under tensile action, the molecular dynamics (MD) method was used to simulate the continuous “tensile failure—self-healing” process, and this study remedies the shortcomings of existing experimental and observational methods. It is found that the MD-reproduced formation process of asphalt binder nanocrack contains four stages: “tensile extension”, “nanocrack generation”, “crack adding, expanding and penetrating” and “cracking failure”. The influence of tensile conditions on the tensile cracking simulation of an asphalt binder model was analyzed, and it was found that low temperature and high loading rate would increase the tensile strength of the asphalt binder model. In addition, the MD-reproduced healing process of asphalt binder nanocracks can be divided into four stages: “surface approach”, “surface rearrangement”, “surface wetting” and “diffusion”, which is similar to the healing process of polymers. Finally, from the perspective of energy change, the change rule of dominant van der Waals energy in the self-healing process was studied. Based on the existing research, the influence of damage degree on the healing performance of asphalt binder and its mechanism were further analyzed. The research results further enrich the theoretical research on microlevel cracking and healing of asphalt materials, and have certain theoretical value for the further development of self-healing asphalt materials.