Copper sulfide (CuS) sorbent exhibits great potential for gaseous elemental mercury (Hg0) decontamination, but it still suffers from a narrow operating temperature. Therefore, designing advanced CuS sorbents that have a high activity level for capturing Hg0 and thermal stability at a high temperature range is challenging. Herein, we propose a metal doping strategy to fabricate a bimetallic sulfide adsorbent. Benefiting the unique structure and composition, a mesoporous structure and an abundance of unsaturated sulfur sites ensure that CuxCo(1–x)Sy provides a desirable level of adsorption for Hg0. The experimental results indicate the optimum Co doping mass concentration of 5 %. The Cu0.95Co0.05Sy not only performs satisfactory Hg0 adsorption at elevated temperatures (Hg0 average adsorption efficiency of over 97.3 %, Hg0 average adsorption rate of over 2.7 μg/g/min), but also presents an exciting regeneration and recycle performance (a Hg0 adsorption efficiency of over 94 % after 10 cycles). The adsorption capacity of Cu0.95Co0.05Sy at the breakthrough threshold of 25 % reaches 5.22 mg/g, surpassing most of metal sulfide sorbents for Hg0 immobilization at 150 °C. As far as Hg0 adsorption is concerned, the composition of typical smelting flue gases has almost no effect. According to further studies, unsaturated coordination short-chain sulfur (S22−) sites are essential for adsorption of Hg0 and are capable of directly forming α-HgS from Hg0. In both the contrast experiment and density functional theory calculations, the cobalt doping strategy enhances the thermal stability of the active S22− ligand and the Hg0 adsorption properties. This study not only provide a prospective adsorbent for Hg0 sequestration at wide temperature range, but also explores a method of utilizing gaseous contaminants for resource utilization.