<p>The novel catalyst had been developed for the efficient treatment of tetracycline (TC) wastewater. The CoFe₂O₄/MoS₂/MIL-101(Fe) material was synthesized by a hydrothermal technique to facilitate the TC degradation by using activated peroxymonosulfate (PMS). The material was subjected to characterizations by SEM, XRD, XPS, and BET. Results proved that a significant quantity of micropores and a substantial specific surface of 82.0463 m²/g of this material could provide more active sites for catalytic activation reaction, and the regeneration cycle of Mo⁴⁺/Mo⁶⁺, Co²⁺/Co³⁺, Fe²⁺/Fe³⁺ of this system could accelerate the electron transfer capacity to enhance the production of reactive radicals, further to improve the TC degradation. The degradation rate of 20&#xa0;mg/L TC could achieve 99.19% within 60&#xa0;min at a catalyst concentration of 0.1&#xa0;g/L, PMS concentration of 0.3&#xa0;g/L, and pH of 3. The CoFe₂O₄/MoS₂/MIL-101(Fe) possessed a stable and stretched crystal structure, after nine cycles of testing, the TC removal rate also reaching 77.53%. The CoFe₂O₄/MoS₂/MIL-101(Fe) might exist three degradation pathways, and SO₄^−· and ·OH played dominant roles in the degradation of TC. This study provided theoretical support for the application for treating the tetracycline wastewater by solving the problem of easy agglomeration, few exposed active sites, and lower internal Fe³⁺/Co³⁺ reduction rate.</p>