The thermo-oxidative aging of Styrene-Butadiene-Styrene (SBS) modified asphalt (SMA) includes the aging of base asphalt and the degradation of SBS modifiers. With the aim of restoring the performance of base asphalt and making up for the loss of performance advantage caused by the degradation of SBS modifier, tall oil and crumb rubber (CR) were applied to synergistically regenerate aged SBS modified asphalt (ASMA). The effect of the particle size and content of CR, as well as the degree of microwave-activated CR on the properties and storage stability of the reclaimed ASMA were discussed in details. The regeneration mechanism of ASMA by CR was studied from the surface properties, morphology and thermal behavior, respectively. The results show that tall oil can restore the low-temperature properties of ASMA significantly, but it seriously detrimental to the high-temperature properties. CR play the role of secondary modification on the reclaimed ASMA, which can improve the high-temperature properties of the reclaimed ASMA at the cost of low-temperature properties and storage stability, and the modification effect is related to the particle size and content of CR. Microwave activation of CR can improve the storage stability of the reclaimed ASMA with CR, which is because that microwave activation modification disrupts the cross-linking structure of the CR and improves the surface properties, which are conducive to the diffusion migration of molecular chains and multiphase material exchange between the CR and the reclaimed ASMA. Thus, the interaction between the multiphases can be enhanced in the reclaimed ASMA with CR. This work provides an effective regeneration method for aged SBS modified asphalt, and also achieves the reuse of non-renewable resources.