In this paper, we prepared CuCo 2 S 4 /MWCNTs as a heterogeneous iron-free bimetal catalyst for the degradation of methylene blue (MB) dye by uniformly synthesizing CuCo 2 S 4 nanoparticles on the surfaces of multiwalled carbon nanotubes (MWCNTs). The homogeneous nanostructure, tuned by MWCNTs, and the efficient electron transfer from CuCo 2 S 4 to MWCNTs resulted in a quite decent catalytic activity, which was superior to that of pristine CuCo 2 S 4 and monometal sulfides. Moreover, CuCo 2 S 4 /MWCNTs maintained a good catalytic performance over a broad pH range of 3 to 12, and exhibited better MB degradation rates under alkaline conditions. Meanwhile, the catalyst was reusable for up to three cycles due to the strong interaction between the nanoparticles and MWCNTs. The results demonstrate that CuCo 2 S 4 /MWCNTs is an improved Fenton catalyst and a promising candidate to substitute iron-based catalysts for the treatment of wastewater containing dyes.