Waste tires can be ground as crumb rubber (CR) and incorporated into asphalt pavement for efficient resource utilization. However, due to its thermodynamic incompatibility with asphalt, CR cannot be uniformly dispersed in the asphalt mix. In order to address this issue, pretreating the CR with desulfurization is a common way to restore some of the properties of natural rubber. The main technique of desulfurization and degradation is dynamic desulfurization, requiring a high temperature that may lead to asphalt fires, aging, and the volatilization of light substances, generating toxic gases and resulting in environmental pollution. Therefore, a green and low-temperature controlled desulfurization technology is proposed in this study to exploit the maximum potential of CR desulfurization and obtain high-solubility “liquid waste rubber” (LWR) close to the ultimate regeneration level. In this work, LWR-modified asphalt (LRMA) with superior low-temperature performance and processability, stable storage, and less susceptibility to segregation was developed. Nevertheless, its rutting and deformation resistance deteriorated at high temperatures. The results showed that the proposed CR-desulfurization technology could produce LWR with 76.9% solubility at a low temperature of 160 °C, which is close to or even better than the finished products produced at the preparation temperature of TB technology, i.e., 220–280 °C.