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[Display omitted] • ECS as a substrate for S-nZVI can effectively avoid agglomeration. • S-nZVI@ECS can effectively remove Cd(II), Cu(II) and Pb(II) in a wide pH range. • The mechanisms include reduction, complexation, and precipitation. • Cu(II) and Pb(II) removal are almost unaffected in the presence of Cd(II). Exhausted copper slag (ECS) is an industrially utilized secondary waste, and due to its large volume and potential environmental risks, the utilization of ECS in a safe manner is required. In this study, a novel synthetic composite (S-nZVI@ECS) was prepared by loading sulfidized nanoscale zerovalent iron (S-nZVI) onto ECS for the removal of Cd(II), Cu(II), and Pb(II) from aqueous solutions. The composite not only provides a new idea for utilizing ECS but also prevents S-nZVI particles from agglomerating. The optimized S-nZVI@ECS can achieve efficient removal of the three heavy metals over a wide pH range without being affected by coexisting ions (Na+, K+, Mg2+, Ca2+). With the respective maximum adsorption capacities of these three cationic heavy metals being as high as 173.01, 93.81, and 338.98 mg/g (based on the Langmuir model), the elimination of S-nZVI@ECS for these three cationic heavy metals could be fitted with the Langmuir and Freundlich models well, and the associated mechanisms (including redox reactions, complexation, and precipitation) were elucidated. The novel S-nZVI@ECS composites prepared in this study using secondary waste as a substrate have good potential for removing cationic heavy metals from aqueous solutions. [ABSTRACT FROM AUTHOR]