A Cu 2+ and Zn 2+ bimetallic doped metal−organic framework Ni 2 (bdc) 2 (dabco) (CuZnNi−MOF, where bdc is 1,4benzenedicarboxylic acid and dabco is 1,4-diazabicyclo[2.2.2]-octane), has been successfully synthesized by the solvothermal method. The carbon-held metal compound nanoparticles (MCN@C) and metal oxide composite (CuOZnONiO) were subsequently obtained by using the CuZnNi−MOF as the precursor. The electrochemical performance of the prepared samples was evaluated in an electrolyte with and without a redox additive (K 4 Fe(CN) 6 ). The specific capacity of the samples tested in the electrolyte with Fe(CN) 6 4− /Fe(CN) 6 3− has a high value of 112.5 mA h g −1 at 1 A g −1 , which is much higher than that measured in the electrolyte without the redox additive, indicating that the Fe(CN) 6 4− /Fe(CN) 6 3− redox couple can effectively enhance the electrochemical performance of electrode materials. An asymmetric supercapacitor (ASC) CuZnNi−MOF//PEDOT-AC (poly(3,4ethylenedioxythiophene)-activated carbon) was further assembled and tested in 3 M KOH + 0.05 MK 4 Fe(CN) 6 electrolyte. The ASC shows a high energy density of 25.2 W h kg −1 , a maximum power density of 8 808 W kg −1 , and also superb cycling performance. Moreover, two assembled ASCs in series connection are found to be able to light up a red light-emitting diode for at least 20 min.