• A CoNC Fenton-like catalyst can efficiently degrade organic pollutants. • It is confirmed that 1 O 2 is the dominant active species for degrading organics. • A CoN 2 C 2 ligands structure has the best catalytic activity for peroxymonosulfate activation. • The generation pathway of 1 O 2 is clearly clarified via DFT calculations. • Electrons can be easily transferred from the organics to peroxymonosulfate. The Fenton-like process shows promising potential to generate reactive oxygen species for the remediation of increasingly environmental pollutants. However, the slow development of high-activity catalysts with strong stability and low leaching of metal ions has greatly inhibited scale-up application of this technology. Here, cobalt (Co)/nitrogen (N) atom co-curved carbon nanorod (CoNC) containing highly uniform CoN x active sites is developed as a Fenton-like catalyst for the effective catalytic oxidation of various organics via peroxymonosulfate (PMS) activation with high stability. As confirmed by the experimental results, singlet oxygen ( 1 O 2 ) is the dominant active species for the degradation of the organics, with a proportion of 100%. Furthermore, density functional theory calculations indicate that CoN 2 C 2 is the most effective ligand structure with more negative adsorption energy for PMS and the shortest length Co–O bond, while the most reasonable generation pathway for 1 O 2 was CoN 2 C 2 –PMS → CoN 2 C 2 –OH* → 2O* → 1 O 2 . Further studies demonstrate that the electron can be transferred from the highest occupied molecular orbitals of the organics to the lowest unoccupied molecular orbitals of the PMS via CoN 2 C 2 action. In addition, the CoNC presents strong resistance to inorganic ions and natural organic matter in the Fenton-like catalysis process. The presence of CoN 2 C 2 active centre can significantly shorten the migration distance of the 1 O 2 generated from PMS activation, which further enhances the Fenton-like catalytic activity in terms of mineralising various organic contaminants with high efficiency over a wide pH range.