Abstract In the present work, SiO2 nanodots were in situ assembled with MgAl-layered double hydroxide (LDH), and the resulting SiO2/LDH nanocomposite was mixed and vulcanized with solution-polymerized styrene butadiene rubber/butadiene rubber (SSBR/BR) to form rubber composites (SiO2/LDH-SSBR/BR). The structure of SiO2/LDH and the resulting rubber composites were characterized by SEM, TEM, high-resolution TEM, XRD, FT-IR, and XPS. It was found that SiO2 nanodots were uniformly dispersed on the surface of LDH, and that the SiO2/LDH was highly compounded with SSBR/BR. With the increasing content of SiO2/LDH, the elongation at break of the SSBR/BR composites increased as much as 600%, while the tensile strength increased gradually and exceeded that of the commercial Zeosil 1165 MP highly-dispersed nano-SiO2 (Zeosil 1165 MP). These results demonstrate the high reinforcing effect of SiO2/LDH-SSBR/BR elastomer composites. Compared with that of Zeosil 1165 MP-SSBR/BR, the tan δ of as-formed SiO2/LDH-SSBR/BR is 48% higher at 0 °C, but 62% lower at 60 °C. Meanwhile, the present SiO2/LDH-SSBR/BR possesses high wet skid resistance and low rolling resistance, and the heat build-up decreases 6.1 °C compared with Zeosil 1165 MP, which provide a promising potential for high-performance green tire applications.