Asphalt pavement will be subjected to the action of thermal, oxygen and ultraviolet during long-term service, which in turn causes the ultraviolet and thermal-oxidative aging of asphalt simultaneously. Based on the long-term aging mechanism, the double retarding effect of surface modified nano-zinc oxide (ZnO) and organic vermiculite (OEVMT) in different stages of long-term aging was utilized in the research. This work investigated the synergistic effect of ZnO and OEVMT on rheological properties and chemical structures of base asphalts (70# and SK-70) and polymer modified asphalts (SBS modified asphalt and SBR modified asphalt) after long-term ultraviolet and thermal-oxidative aging. Dynamic shear rheological (DSR), bending beam rheological (BBR) and Fourier infrared spectroscopy tests were utilized to study the DSR properties, BBR properties at low temperature and chemical structures, respectively. Meanwhile, the synergistic effect mechanism was analyzed. Results showed that the effect of 1 % ZnO to resist the long-term ultraviolet aging of 70# base asphalt approximates that of 3 % OEVMT, while the long-term thermal-oxidative anti-aging ability of 1 % OEVMT for 70# base asphalt is equivalent to that of 3 % ZnO. Besides, compared with 2 % ZnO or 2 % OEVMT, 1 % ZnO + 1 % OEVMT shows a better long-term ultraviolet and thermal-oxidative aging resistance for different asphalt binders, indicating its synergistic effect in strengthening the anti-aging performance of asphalt. Moreover, 1 % ZnO + 1 % OEVMT not only can effectively retard the oxidation rate of asphalt in the process of long-term aging, but also inhibit the degradation degree of modifiers in SBS modified asphalt. The research could propose a new design idea to effectively solve the long-term aging problem of asphalt.