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Cobalt‐based catalysts are widely used as efficient activator for the activation of peroxymonosulfate (PMS). A new carbon enclosed magnetic metal cobalt (Co@C) catalyst was successfully synthesized by high‐temperature pyrolysis of cobalt‐based metal‐organic framework. The prepared Co@C catalyst demonstrated remarkable catalytic activity for the degradation of contaminants (99.9 % for tetracycline (TC) degradation within 10 min). The TC degradation efficiency could still sustain more than 99 % after three cycles. Moreover, the Co@C/PMS system exhibited great universality for the rapid removal of other dyes such as methyl orange (MO) and methylene blue (MB). The zero‐valent cobalt was engaged in the activation of the PMS and reacted with O2 to form Co2+, to make sure that there was enough Co2+ to activate PMS to generate Co3+. Simultaneously, the produced Co3+ ions extracted electrons out of HSO5- ${{{\rm { HSO}}}_{{\rm { 5}}}^{{\rm { -}}}}$ , driving a Co0/Co2+/Co3+ circulation to keep the high efficiency for rapid degradation of TC. In summary, this work offers a novel strategy to develop an effective magnetic heterogeneous catalyst to activate PMS for the elimination of difficult to degrade contaminants. [ABSTRACT FROM AUTHOR]