<p>Molybdenum disulfide (MoS₂) presents considerable potential as an electrode material for supercapacitors, but its inert basal plane hinders the activation of electronic states and limits electrochemical performance. To overcome this challenge, we developed and successfully synthesized a novel layered nanocomposite (Ni-intercalated 1T-MoS₂) using an exfoliation-reassembly method. Consequently, the distribution of Ni cations within the interlayer space of the 1T-MoS₂ lattice is examined through X-ray diffraction, Raman spectroscopy and transmission electron microscopy (TEM). As a result, a highly porous structure has been achieved due to adequate intercalation of Ni ions as confirmed by Langmuir specific surface area measurements. Besides, the electrochemical results of our Ni/1T-MoS₂ strongly embark on benefits of layered composite structure for the charge storage kinetics. At a current density of 0.5 Ag^− 1, the Ni/1T-MoS₂ composite showed remarkable synergistic qualities, obtaining a high specific capacitance of 1488 Fg^− 1. After 5000 cycles, the Ni/1T-MoS₂ composite maintained 95.14% of its capacitance, demonstrating exceptional cycling stability. Furthermore, the asymmetric device, which combines porous Ni/1T-MoS₂ with activated carbon, displayed outstanding energy density (95.14 Wh kg^− 1 at 914 Wkg^− 1) and excellent cycling stability (92.1% capacitance retention after 5000 cycles). The successful operation of LEDs highlights the Ni/1T-MoS₂ (0D/2D) composite’s potential for high-energy storage applications.</p>