With the huge production of natural rubber (NR), it is feasible to produce natural rubber–modified asphalt binder (NRMB) to achieve carbon neutrality and environmental sustainability in asphalt pavement construction. As a solid thermoplastic elastomer, the dispersion and compatibility of NR in the asphalt binder are poor, which is the main obstacle to using these solid thermoplastic elastomers as modifiers. Accordingly, a high-performance vulcanized natural rubber–modified asphalt binder (VNRMB) was prepared by rotational shearing to disperse NR into the asphalt binder, providing the modification scheme of NR and optimizing the performance of the modified binder to be conducive the better durability. First, the best vulcanization scheme was determined by the consistency tests. Then the rheological and low-temperature properties of the asphalt binders were tested by the dynamic shear rheometer (DSR) and bending beam rheometer (BBR) tests, respectively. It was found that in high and low temperatures, VNRMB performed significantly better than virgin asphalt binder (VB) and NRMB. The high-temperature deformation resistance and low-temperature cracking resistance for 2.5/10VNRMB were significantly better than those of 2.5NRMB and VB, apart from the lower thermal sensitivity, the better elastic recovery, and storage stability. Fluorescence microscopy (FM) and Fourier transform infrared spectroscopy (FT-IR) tests indicated that NR dispersed in the binder was cross-linked by the sulfur to form a network structure in VNRMB. In general, the novel VNRMB prepared in this paper exhibits preferable performance. Compared with VB and NRMB, VNRMB has better elastic recovery, rutting resistance, and low-temperature cracking resistance. Using VNRMB on the top layer is suggested because of the preferable rutting resistance, but the thermal cracking caused by extreme temperature gradients should be further studied and pursued. Additionally, for cold areas, using VNRMB on the intermediate or bottom layers is suggested to improve low-temperature cracking resistance. However, these results were only from preliminary tests of asphalt binders. In the future, the pavement performances of the modified asphalt mixture, including rutting and fatigue cracking, should be studied with different states of vulcanization of VNRMB considered. Moreover, in the process of study, it was found that the mild cross-linking state could maximize the ductility of modified asphalt binders. But the low-temperature performance of the asphalt mixture was not proved as the best. It is also necessary to conduct further study on the pavement performance of the modified asphalt mixture with different states of vulcanization. [ABSTRACT FROM AUTHOR]