The high capacitive, cost-effective, non-toxic nickel.cobalt layered double hydroxide nanofoam pseudocapacitive electrode materials doped with aluminium (NiCoAl-LDH) have been hydrothermally synthesized on the electrochemically modified graphite (G) substrate with zinc and copper (Zn/G and Cu/ Zn/G). The Al3+ diffusion in the LDH during the hydrothermal synthesis resulted in an ultrathin nanofoam morphological structure well adapted to the entire surface of Zn/G and Cu/Zn/G. The high areal capacitance of the best efficient NiCoAl-LDH/Cu/Zn/G electrode of 2.17 F cm-2 at 5 mA cm-2 decreases to 1.83 mF cm-2 at 75 mA cm-2 showing an excellent rate capability of 84%. An asymmetric supercapacitor (ASC) designed with graphite as negative electrode exhibits an energy density of 29.3 Wh kg-1 at a power density of 575 W kg-1. It still remains at 5.6 Wh kg-1 at a higher power density of 3477 W kg-1 at a discharge time of 5.8 s indicating ultra-fast energy storage ability of the G//NiCoAl-LDH/Cu/Zn/G device. Its cyclic tests were also made by constructing a coin-cell-type device for industrial applications. The capacitance of the coin-cell operating within 1.6 V was protected around 100% even after over 10,000 charge.discharge cycles at the current densities up to 1.8 mA cm-2.