With the aim of rejuvenating the excellent performance of aged SBS modified asphalt, colza oil bio-asphalt (COA) and polymethylene polyphenyl isocyanate (PAPI) were used in this study for adjusting the asphalt components and repairing SBS molecular structure, respectively. The above-mentioned dual regeneration mechanism was verified by comparing the effects of different rejuvenation components on the physical and rheological properties as well as molecular weight distribution of short-term aged SBS modified asphalt. Also, according to the change law of rheological performance of un-aged base asphalt and SBS modified asphalt with the effect of dual regeneration agent, the influence of rejuvenator itself on the phase angle platform area was excluded. Under the comprehensive consideration of the physical and rheological properties of dual recycled SBS modified asphalt, the optimal dosage of COA and PAPI was determined. The experimental results indicate that the double regenerant can not only regulate the asphalt components, but also connect the SBS molecular structure, resulting in restoring the physical and rheological performance of aged SBS modified asphalt. The optimal ratio of the dual regenerant is determined to be 12 wt% COA and 1.25 wt% PAPI. In addition, the fluorescence microscopy test results further verifies that PAPI has the ability to rebuild the SBS network structure.