Cobalt-based heterogeneous nanocatalysts have attracted much attention in activating persulfate to rapidly eliminate organic pollutant in water. However, it remains a challenge to realize the easily recovery of these nanocatalysts and reduce the leaching of Co ions. Herein, Co@C core-shell nanostructures are anchored on the surface of carbon cloth (CC). The as-obtained immobilized catalyst of Co@C/CC exhibits an enhanced catalytic activity and lower leaching of Co ions in comparison with the bare Co@C nanocatalyt because of the high electrical conductivity and carrier effect of CC. The Co@C/CC demonstrates efficient catalytic performance in activating peroxymonosulfate (PMS) for tetracycline (TC) degradation. 99% of TC can be quickly degraded by the Co@C/CC/PMS system, and the system has good durability and interference resistance as well as wide pH adaptability from 3 to 10. Scavenger quenching experiments and electron paramagnetic resonance (EPR) shows that the non-free radical pathway (1O2) is dominate contribute to the TC degradation. Finally, density functional theory (DFT) calculations yield CC as the primary attack site in TC, and the possible degradation pathways of TC are inferred. Importantly, the immobilized catalyst of Co@C/CC can achieve fast and simple collection and regeneration. This work provides new ideas for the preparation of efficient catalysts with easily recyclable for rapidly eliminate organic pollutant in water.