The development of low-cost and highly efficient adsorbents is essentially needed for removing Hg2+ species from desulfurization sludge leaching wastewater. In this study, a series of novel Cu-modified attapulgite (Cu-ATP) adsorbents were synthesized via a simple HNO3 treatment combined with an improved impregnation method. The Hg2+ removal efficiency of these Cu-ATP adsorbents was investigated in simulated leaching wastewater. The effects of HNO3 concentration, Cu precursor, Cu loading content, and other adsorption conditions on Hg2+ removal using Cu-ATP were investigated. The results demonstrated that Cu-ATP prepared with CuSO4 as the precursor and treated with 3 mol/L HNO3 showed excellent Hg2+ removal performance. Moreover, with increasing adsorbent content and adsorption time, the Hg2+ removal efficiency of Cu-ATP first increased and then stabilized. However, with an increase in pH value, the Hg2+ removal efficiency first increased and then decreased, whereas the removal showed a decreasing trend with increasing initial Hg2+ concentration. The adsorption kinetics results indicated that Hg2+ adsorption on Cu-ATP was well described by the pseudo-second-order model. Furthermore, various characterization methods, including Brunauer − Emmett − Teller analysis (BET), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS), were employed to analyze the physicochemical properties of the adsorbents. The analyses confirmed that the superior Hg2+ removal efficiency of Cu-ATP was mainly due to the complexation of Hg2+ with chemisorbed oxygen produced by Cu doping and S species generated from the Cu precursor (CuSO4). These findings underscore the potential of Cu-ATP as a cost-effective adsorbent for removing Hg2+ from wastewater.