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To explore advanced oxidation catalysts, peroxymonosulfate (PMS) activation by Co-Ni-Mo/carbon nanotube (CNT) composite catalysts was investigated. A compound of NiCo₂S₄, MoS₂, and CNTs was successfully prepared using a simple one-pot hydrothermal method. The results revealed that the activation of PMS by Co-Ni-Mo/CNT yielded an exceptional Rhodamine B decolorization efficiency of 99% within 20 min for the Rhodamine B solution. The degradation rate of Co-Ni-Mo/CNT was 4.5 times higher than that of Ni-Mo/CNT or Co-Mo/CNT, and 1.9 times as much than that of Co-Ni/CNT. Additionally, radical quenching experiments revealed that the principal active groups were ¹O₂, surface-bound SO₄^•−, and •OH radicals. Furthermore, the catalyst exhibited low metal ion leaching and favorable stability. Mechanism studies revealed that Mo⁴⁺ on the surface of MoS₂ participated in the oxidation of PMS and the transformation of Co³⁺/Co²⁺ and Ni³⁺/Ni²⁺. The synergism between MoS₂ and NiCo₂S₄ reduces the charge transfer resistance between the catalyst and solution interface, thus accelerating the reaction rate. Interconnected structures composed of metal sulfides and CNTs can also enhance the electron transfer process and afford sufficient active reaction sites. Our work provides a further understanding of the design of multi-metal sulfides for wastewater treatment.