SBS-modified bitumen (SMB) is susceptible to aging, which seriously influences its service performance and life. In order to strengthen the anti-aging ability of SMB, triethoxyvinylsilane was designed to organically modify layered double hydroxides (LDHs) and was applied to modify SMB. The dispersibility and storage stability of LDHs in SMB were markedly enhanced after triethoxyvinylsilane organic modification, and the compatibility and storage stability of SBS in bitumen were simultaneously enhanced. Compared with SMB, the introduction of LDHs and organic LDHs (OLDHs) could ameliorate the high-temperature properties of SMB, and the thermostability of SBS in bitumen at a high temperature was also distinctly improved, especially OLDHs. After aging, due to the oxidation of molecular bitumen and the degradation of molecular SBS, SMB became hardened and brittle, and the rheological properties were significantly deteriorated, which had serious impacts on the performance of SMB. LDHs can mitigate the detriment of aging to bitumen and SBS, and the deterioration of the rheological properties of SMB is obviously alleviated. As a result of the better dispersibility and storage stability, OLDHs exerted superior reinforcement of the anti-aging ability of SMB.