A series of (Fe2.2Mn0.8Cux)1−δO4 (x=0, 0.2, 0.5, and 0.8) was synthesized for elemental mercury capture. The as-synthesized adsorbents were characterized by Brunauer–Emmett–Teller (BET), powder X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The experimental results show that (Fe2.2Mn0.8Cu0.5)1−δO4 catalyst adsorbent exhibits the best elemental mercury capture capacity with the increase in mercury removal efficiency by 20% as compared to the (Fe2.2Mn0.8)1−δO4 adsorbent. The XPS results indicate Cu dopant can provide the lattice oxygen on the adsorbent surface due to the transformation from Cu2+ cations to Cu+ cations, which increases the active sites for elemental mercury adsorption. The Mn4+ cations on the adsorbent surface may oxidize the adsorbed mercury to mercury oxidization. Meanwhile, the Mn3+ cations formed are also oxidized to the Mn4+ cations by the gaseous oxygen phase in the reactor gas. However, the large Cu content may block the collision between Mn4+ cations and adsorbed mercury, and thus decrease the oxidization capability of adsorbent surface for mercury. Therefore, the Cu dopant with the suitable content may be a potential modified method for the adsorbent to further increase the elemental mercury capture.