Although Fenton or Fenton-like reactions have been widely used in the environment, biology,life science,and other fields,t he sharp decrease in their activity under macroneutral conditions is still al arge problem. This study reports aM oS 2 cocatalytic heterogeneous Fenton (CoFe 2 O 4 /MoS 2 )s ystem capable of sustainably degrading organic pollutants,s uch as phenol, in am acroneutral buffer solution. An acidic microenvironment in the slipping plane of CoFe 2 O 4 is successfully constructed by chemically bonding with MoS 2 .T his microenvironment is not affected by the surrounding pH, which ensures the stable circulation of Fe 3+ /Fe 2+ on the surface of CoFe 2 O 4 /MoS 2 under neutral or even alkaline conditions. Additionally,C oFe 2 O 4 /MoS 2 always exposes "fresh" active sites for the decomposition of H 2 O 2 and the generation of 1 O 2 , effectively inhibiting the production of iron sludge and enhancing the remediation of organic pollutants,even in actual wastewater.T his work not only experimentally verifies the existence of an acidic microenvironment on the surface of heterogeneous catalysts for the first time,but also eliminates the pH limitation of the Fenton reaction for pollutant remediation, therebye xpanding the applicability of Fenton technology.