Based on the electrochemical mechanism of Faraday supercapacitors (FSs), we design a microstructure configuration of electrode materials (EMs) in this work, aiming to promote the electrochemical performance of FSs. This configuration of EMs has two dimensional sheets-crosslinked network with narrow mesopore size distribution. It is reasonable to believe that the configuration is in favor of the electrochemical performance of EMs to the greatest extent. We try to build this structure configure using Ni-Co layered double hydroxide (LDH) nanosheets as building blocks by a facile sol-gel approach. Due to the Co2+ ions, we realize this structure configuration consisting of Ni-Co LDH nanosheets. Benefiting from the advantages of this configuration, the Ni-Co LDH presents high electrochemical performance. It has high specific capacity of 1170 C g(-1) at low current density of 2.0 A g(-1), and 500 C g(-1) at high current density of 39.6 A g(-1). The asymmetric supercapacitors of Ni-Co LDH exhibit high energy density of 74.37 Wh kg(-1) at low power density of 492 Wh kg(-1) and keep relatively high energy density of 15.99 Wh kg(-1) at high power density of 6395 Wh kg(-1). These results suggest that the designed structure configuration of EMs is rational for application in FSs. (C) 2019 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved.