1-Naphthylthiocarbamide (ANTU) doped xerogel was prepared and investigated for removal of mercury ions from aqueous media. Physicochemical parameters such as effect of pH, equilibration time, and adsorption isotherm on the removal of mercury were evaluated to optimize the conditions to utilize the data on a large scale. It was observed that uptake and retention of mercury ions inside the pores take place by the formation of a complex with the entrapped reagent molecules. The data show that a xerogel doped with 0.2 mmol ANTU/g of sorbent can remove 0.096 mmol Hg. The probable composition of the mercury complex has been deduced and a removal mechanism is suggested. The regeneration and reuse of doped gel for the removal of targeted metal has been discussed.