Layered double hydroxides (LDH) as active electrode materials have become the focus of research in energy storage applications. The manufacturing of excellent electrochemical performance of the LDH electrode is still a challenge. In this paper, the production of CoAl-LDH@Ni(OH)2 is carried out in two steps, including hydrothermal and electrodeposition techniques. The prominent features of this electrode material are shown in the structural and morphological aspects, and the electrochemical properties are investigated by improving the conductivity and cycle stability. The core of this experimental study is to investigate the properties of the materials by depositing different amounts of nickel hydroxide and changing the loading of the active materials. The experimental results show that the specific capacity is 1810.5F · g−1 at 2 A/g current density and the cycle stability remained at 76% at 30 A g−1 for 3000 cycles. Moreover, a solid-state asymmetric supercapacitor with CoAl-LDH@Ni(OH)2 as the positive electrode and multi-walled carbon nanotube coated on the nickel foam as the negative electrode delivers high energy density (16.72 Wh kg−1 at the power density of 350.01 W kg−1). This study indicates the advantages of the design and synthesis of layered double hydroxides, a composite with excellent electrochemical properties that has potential applications in energy storage. © The Author(s) 2018. Published by ECS. This is an open access article distributed under the terms of the Creative Commons Attribution 4.0 License (CC BY, http://creativecommons.org/licenses/by/4.0/), which permits unrestricted reuse of the work in any medium, provided the original work is properly cited. © The Author(s) 2018. Published by ECS.