In recent times, there has been a significant focus on research into the creation of an environmentally sustainable and pollution-free hydrogen storage cell power system. Over the last ten years, a number of significant advancements in energy storage methods have been developed, impacting research, innovation, and the likely course for furthering our understanding of energy storage. We suggest a hydrogen energy storage device built using cutting-edge electrochemical techniques and electrode materials. As active materials, a range of nanocomposites based on gadolinium aluminate (Gd4Al2O9) and carbonous compounds were created. For the fabrication of Gd4Al2O9 nanostructures, ultrasonic radiation was used in the presence of Schiff-base ligands of N,N′-bis(salicylidene)ethylenediamine (H2Salen), N,N0-disalicylidene-1,4-di-aminobutane (H2Salbn) and N,N′-bis(salicylidene)-1,2-phenylenediamine (H2Salophen). Diverse carbon-based materials of g-C3N4, GO and CNT were utilized for designing nanocomposites. After 15 cycles, the hydrogen storage capacities of pure Gd4Al2O9 were found to be 121 mAhg−1. Then, in the fifteenth cycle, the nanocomposites' capacity rose to 278 mAhg−1 at a current of 1 mA for designed nanocomposite with GO. The CNT can increase the capacity to 302 mAhg−1 (11th cycle) but the fading capacity was occurred after 11th cycle to 112 (15th cycle). The g-C3N4 led to decrease in capacity due to blocking the pore and active sites of Gd4Al2O9 nanostructures.