To comprehensively reuse the leaching residue obtained from lead-zinc tailings, an active silicon adsorbent (ASA) was prepared from leaching residue and studied as an adsorbent for copper(II), lead(II), zinc(II), and cadmium(II) in this paper. The ASA was prepared by roasting the leaching residue with either a NaCO/residue ratio of 0.6:1 at 700 °C for 1 h or a CaCO/residue ratio of 0.8:1 at 800 °C for 1 h. Under these conditions, the available SiO content of the ASA was more than 20%. The adsorption behaviors of the metal ions onto the ASA were investigated and the Langmuir, Freundlich, and Dubinin-Radushkevich isotherm models were used to analyze the adsorption isotherm. The result showed that the maximum adsorption capacities of copper(II), lead(II), cadmium(II), and zinc(II) calculated by the Langmuir model were 3.40, 2.83, 0.66, and 0.62 mmol g, respectively. The FT-IR spectra of the ASA and the mean free adsorption energies indicated that ion exchange was the mechanism of copper(II), lead(II), and cadmium(II) adsorption and that chemical reaction was the mechanism of zinc(II) adsorption. These results provide a method for reusing the leaching residue obtained from lead-zinc tailings and show that the ASA is an effective adsorbent for heavy metal pollution remediation.