An increase in heavy metal contamination in aquatic environments require an efficient sorbent for the removal and reuse of toxic elements. We attempted to synthesize arginine/lysine-functionalized MgAl LDHs in one-pot without using any hazardous alkaline reagents. The LDHs produced at lower temperatures showed larger numbers of amino acids on their surfaces, while these are exchanged with CO32- at higher temperatures. The arginine/lysine present on the surface of LDH enhanced the adsorption of Co2+ and showed the highest adsorption capacity of 1.159 and 1.170 mmol/g for the LDHs functionalized with lysine and arginine, respectively. Kinetics studies indicated that the adsorption of Co2+ occurred by multiple mechanisms. The Co2+ adsorption on these amino acid functionalized LDHs occurs by the formation chelation complex with amino acid, which provide better vicinity of Co2+ to basic LDH that facilitating the enhanced immobilization. The sorption of other divalent metal ions on these arginine/lysine functionalized LDHs followed the order of Co2+ > Ni2+ > Mn2+ > Fe3+. The Co2+ forms diamine-like coordination that is stable on the surface of LDH and causes higher sorption densities, while other metals form partial glycine-like coordination that detaches the amino acid from the surface of LDH, thereby leading to lesser sorption capacity. The conversion of anionic LDH in to a cationic sorbent was successfully fabricated by these arginine/lysine-assisted methods and explored for the remediation of Co2+ from aqueous solution.