In this work, MoS2 is utilized as a cocatalyst to enhance Fe3+/PMS reaction for the deep oxidation of aromatic VOCs in a continuous air-bubbling system. The exposed Mo4+ active sites achieve high-speed electron transfer from MoS2 (001) surface to Fe3+ and accelerate Fe2+ regeneration (~60%), which greatly promotes O2 and PMS activation for the formation of radicals like O-2(center dot-), HO center dot and SO4 center dot-. Consequently, the Fe3+/PMS/MoS2 system exhibits strong catalytic ability for various VOCs degradation including styrene, toluene and chlorobenzene (with removal efficiency of 97%, 84% and 83%, respectively) at a wide pH range (3-9). MoS2 cocatalyst in Fe3+/PMS reaction greatly promotes the activation of O-2 into radicals and inhibits the formation of toxic aromatic byproducts via the deep oxidation of styrene into CO2. Our study provides a green strategy to activate O-2 for pollutants degradation and has great potential to be widely applied in actual environment remediation.