The two-step surface modifications of activated carbon was carried out to improve the adsorption capacity of toxic heavy metal ions in liquid phase. Physical and chemical properties of the as-received activated carbon (AC) and two kinds of surface-modified activated carbons (1stAC and 2ndAC) were evaluated through the BET analysis, surface acidity, and oxides measurements. Specific surface area and pore volume did not significantly change, but surface oxide-group remarkably increased by the surface modification. Equilibrium and batch adsorptions of the various metals, such as Pb, Cd, and Cr, using AC, 1stAC, and 2ndAC were performed at initial pH 5. The adsorption capacity and rate of 2ndAC were higher than those of AC and 1stAC. The carboxylic/sodium carboxylate complex groups were developed from the two-step surface modification of activated carbon, which strongly affected the adsorption of metal ions.