Two-dimensional graphene oxide (GO) nanosheets with high electrical conductivity and electrochemical stability are employed as a hybridization matrix to improve the electrode performance of layered double hydroxides (LDHs). A cobaltchromium-LDH hybridized with a GO matrix leads to anchored Co-Cr-LDH-GO (CCG) self-assembly with a high surface area, mesoporous morphology, high electrical conductivity, and high charge transfer kinetics. The CCG nanohybrids display enhanced specific capacity (1502 C g −1 ) with high-rate characteristics compared to pristine Co-Cr-LDH (591 C g −1 ), signifying the crucial role of GO as a hybridization matrix for improving the electrode performance of LDH materials. Aqueous and all-solid-state hybrid supercapacitors are fabricated using the best-optimized CCG nanohybrid and reduced graphene oxide as an anode and a cathode, respectively. The aqueous device delivers a specific capacitance of 181 F g −1 , a specific energy (SE) of 56.66 Wh kg −1 , and a specific power (SP) of 600 W kg −1 at 0.8 A g −1 . Moreover, the solid-state device delivers a specific capacitance of 130.8 F g −1 , a SE of 46.50 Wh kg −1 , and a SP of 1536 W kg −1 at 1.92 A g −1 . The present study clearly demonstrates the usefulness of conducting GO as an efficient hybridization matrix to improve the electrode performance of LDHs.