Fenton technology is promising for removing recalcitrant and toxic organic contaminants for wastewater purification. Neutral Fenton technology is preferred for its reduced acid usage and improved operational convenience. However, the challenges are the low production of reactive species and the limited conversion of high-valent iron (Fe) to low-valent Fe. This study introduced a new cycle employing high-valent iron-oxo species [Fe(IV)=O], which directly participates in degradation, facilitating Fe regeneration. To achieve it, we developed an O-doped single Fe atom catalyst (SACs, Fe-N