Atomic-layered α-V 2 O 5 nanosheets with a thickness of 5−7 layers were synthesized successfully via a fast gas-driven exfoliation process. The main advantages of this method are its more facile operation procedures, shorter preparation time, and higher yield. The obtained α-V 2 O 5 nanosheets exhibit an enhanced aerobic oxidative desulfurization ability obviously. Sulfur removal of dibenzothiophene could reach up to 99.7% (less than 2 ppm) under optimized conditions.