Layered double hydroxide intercalated with tartrate (tartrate-Mg-Al) was used as an adsorbent to remove lead ions from aqueous solutions. The effects of various optimization parameters such as contact time, solution pH, lead ion concentrations, and adsorbent dosage were investigated by the use of Response Surface Methodology (RSM). The Response Surface Methodology (RSM) based on a four-level four-variable Central Composite Rotatable Design (CCRD) was employed to evaluate the interactive effects of the various optimization parameters. The parameters were contact time (6–10 h), solution pH (1–3), adsorbent dosage (0.06–0.1 g), and lead ion concentrations (10–30 mg/L). The percentage of lead ions removal for each of the parameters studied was determined by Inductively Coupled Plasma-Optical Emission Spectrophotometer. Simultaneously by increasing contact time and amount of dosage of tartrate-Mg-Al used the percentage of lead ions removal from aqueous solution will increase; however, the percentage removal decreases with an increase in pH and concentrations of lead ions. The experimental percentage removal recorded under optimum conditions was compared well with the maximum predicted value from the RSM, which suggest that Central Composite Rotatable Design of RSM can be used to study the removal of lead from aqueous solution by the use of tartrate-Mg-Al as an adsorbent.