High-efficient-adsorbents-layered double hydroxides (LDH) intercalated by carbonate ion and ethylenediaminetetraacetic acid (EDTA) ion were synthesized bythe coprecipitation method for the removal of Ni2+ in theaqueous solution. MgAl−EDTA−LDH had a better adsorption performance than MgAl−CO3−LDH due to the largerspecific surface area and strong trapping for heavy metal ionsof EDTA. Ni(II) adsorption on the two kinds of LDHconformed to the pseudo-second-order kinetic model. TheLangmuir isothermal adsorption model was more suitable todescribe the adsorption isotherm than the Freundlich model. The maximum adsorption capacity of MgAl−EDTA−LDH andMgAl−CO3−LDH for Ni(II) was 108.2 and 23.47 mg/g, respectively. This work may offer ideas for the preparation andapplication of excellent adsorbents in the heavy metal removal from polluted water.