This work aimed to study the synthesis of Mg/Al layered double hydroxides (LDH) from aluminum residues. LDH was produced by co-precipitation and hydrothermal methods using Al(OH)3 synthesized from aluminum residue. It was possible to confirm the formation of LDH, with an increase in crystallinity for the hydrothermal synthesis. The FTIR indicates no influence regarding the Al(OH)3 origin (synthesized or commercial). N2 adsorption/desorption isotherms indicate a mesoporous structure with non-rigid aggregates of plate-shaped particles creating slit pores of varying shapes and sizes. The synthesized materials presented surface area ranging from 27.66 to 96.08 m2/g and pore diameter between 20 and 500 Å. Finally, it can be affirmed that LDHs were satisfactorily synthesized using aluminum residue as a source of aluminum hydroxide.