The iron-based materials are commonly applied as catalysts in the advanced oxidation processes since they have high-activity and are pollution-free to the environment. How to minimize the continuous depletion of Fe2+ and maintain high-activity is now a hot issue. Herein, a FeOOH@MoS2 catalyst was prepared to activate peroxymonosulfate to efficiently degrade Atrazine (ATZ). The results showed that FeOOH@MoS2 exhibits excellent catalytic activity allowing ATZ to be degraded by up to 97.90 % in 60 min. On the one hand, the Fe2+ in FeOOH can efficiently activate the PMS to generate active species to degrade the ATZ, on the other hand, MoS2 accelerates the reduction of the generated Fe3+ to Fe2+, allowing FeOOH@MoS2 to maintain high activity. Radical quenching and electron paramagnetic resonance (EPR) tests show that •OH and sulphate radical played predominant roles in the advanced oxidation process. FeOOH@MoS2 catalyst showed a good stability, with only a 10.1 % decrease in ATZ degradation after 5 cycles. This work provides a new strategy to fabricate iron-based catalysts for more efficiency in PMS activation.