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CoZn layered double hydroxide (LDH) or Co(OH)2 pseudocapacitive material has been prepared on the current collector of carbon fiber paper (CFP) using an eco-friendly one-step electrodeposition. Benefiting from its unique structural feature, the binder-free CoZn LDH/CFP electrode material realizes high specific capacitance of 1156 Fg−1 at a current density of 1 Ag−1 and excellent rate capability of 80% retention with 16 fold current density increment, which is much better than that of Co(OH)2 (617 Fg−1, 65%). Notably, the CoZn LDH/CFP can retain an outstanding electrochemical stability with a capacitance degradation of only 6% after 6000 charge–discharge cycles at 32 Ag−1. Moreover, an asymmetric supercapacitor (ASC) using CoZn LDH/CFP as a positive electrode and AC/CFP as a negative electrode has been assembled. The ASC exhibits a superior energy density of 30.0 Whkg−1 at a power density of 800 Wkg−1 with a specific capacitance up to 84.4 Fg−1 and a potential window wide to 1.6 V. These encouraging results indicate that CoZn LDH/CFP composite material has a great potential for next-generation energy conversion/storage devices. [ABSTRACT FROM AUTHOR]