Electrodes of Ni/Al layered double hydroxide (Ni/Al LDH) coated on the surface of nickel foam are successfully prepared by an in situ method using a mixed aqueous solution of nickel nitrate and aluminum. Their structure and surface morphology are studied by X-ray diffraction and scanning electron microscopy analysis. Their supercapacitance performances are investigated by cyclic voltammetry and constant current charge/discharge measurements. Results show that Ni/Al LDH nanoplatelets densely cover the nickel foam substrate. The electrode shows excellent electrochemical capacitive character and displays a specific capacitance of 701 F g−1 at a current density of 10 mA cm−2. The capacitance loss is less than 6% after 400 charge−discharge cycles. The larger contact area between the nickel foam supporter and active materials greatly enhances the use of Ni/Al LDH.