Recently, Fe-based materials have been widely used to activate persulfate (PMS) for the degradation of organic pollutants. However, the sluggish Fe(III)/Fe(II) cycle often results in catalyst deactivation. In this work, we modified iron oxide on carbon nitride with molybdenum (FeMo/CN), which was characterized by the interfacial sites of Fe0/Fe2(MoO4)3 and Fe2O3/Fe2(MoO4)3. Systematic investigations indicate that the interfacial sites in the FeMo/CN material promote the cycling efficiency of Fe(III)/Fe(II). Also, the strong interaction between FeMo/CN and PMS drives the transformation of PMS into O2•-, which subsequently undergoes conversion to form 1O2 as the main reactive oxygen species. 50 mg·L-1 Rhodamine B (RhB) can be almost completely removed within 20 min in the FeMo/CN + PMS system. The FeMo/CN catalyst suppresses the majority of catalysts documented in previous studies, showing an impressive specific rate constant value of 10.78 L2·min-1·g-2. Additionally, the FeMo/CN + PMS system demonstrates remarkable wide-ranging applicability, excellent environmental tolerance, and good stability. It has the capacity to continuously treat 51.84 L of simulated organic pollutants (RhB solution) while consistently maintaining a degradation rate of over 99%. This work highlights the practicality of interface engineering in Fe-based materials and inspires the rational design of materials for sustainable environmental remediation.