The synergistic effect between mixed metal sulfides and bimetallic layered double hydroxides (LDHs) is pivotal for their refined energy storage capacities owing to their unique biomimetic-designed 3D Asteraceae flower-like intercalated layered heterostructures. Herein, we report a high-performance MoS 2 / Ni 3 S 4 @NiCr-LDH41 mesoporous heterostructure fabricated via a two-step hydrothermal reaction. This biomimetic-designed 3D Asteraceae flower architecture exhibits a dominant battery type (pseudocapacitance) charge storage mechanism, further authenticated by electrochemical studies. The mesoporous interconnected wall structure offers a colossal specific capacitance of 2323.33 F g −1 at a 0.5 A g −1 current density. Furthermore, the symmetric and asymmetric supercapacitor devices are designed to explore their electrochemical performance. The symmetric assembly exhibits the highest specific capacitance of 111.45 F g −1 at a current density of 1 A g −1 with a capacitance retention of 81.73% over 5000 continuous charge−discharge cycles. It delivers an energy density of 22.29 Wh kg −1 at a power density of 1200 W kg −1 . Markedly, the asymmetric configuration MoS 2 /Ni 3 S 4 @NiCr-LDH41||AC provides the highest specific capacitance of 71.37 F g −1 at 1 A g −1 current density with energy and power densities of 25.37 Wh kg −1 and 800 W kg −1 , respectively, and stupendous electrochemical stability over 10,000 (85.01% capacitance retention) charge−discharge cycles. For the demonstration of real-time applications, two devices are connected in series, which allows the illumination of green LED light for symmetric (90 s) and asymmetric devices (200 s). These favorable outcomes accentuate the magnificent electrochemical performance within the potential and viability of Asteraceae flower−architectured MoS 2 /Ni 3 S 4 @NiCr-LDH41 heterostructure as an electrode material for high-performance supercapacitors.
