Developing an economic and efficient approach for the production of adipic acid is a grand challenge in the chemical industry. Toward this goal, we report a simple method for selective synthesis of adipic acid from cyclohexane with NO2 by using Ni-Al-VPO/MCM-41 as catalyst. The physical-chemical properties of supported Ni-Al-VPO/MCM-4 catalysts were characterized, the reaction conditions were optimized, and the reusability of the catalyst was examined. The results showed that the supported 30%Ni-Al-VPO/MCM-41 catalyst exhibited excellent catalytic performance with 65.1% of cyclohexane conversion and 85.3% of selectivity toward adipic acid, especially, its catalytic performance was still stable after five runs. Maybe this developed method has potential industrial application prospects for production of adipic acid.