Energy from hydrogen has been looked upon with great favours to encounter the shortage of fossil fuels in energy generation. Safety issues and storage concerns of hydrogen has been a major drawback in this regard. Here, a novel material g–C3N4–MoS2–Ni(OH)2 is crafted to achieve promisingly sufficient storage capacity for hydrogen. Hydrothermal route is optimized in a best possible way to achieve flower like structure of MoS2. It is then blended with fine sheets of Ni(OH)2 and as synthesized g-C3N4 to develop the promising nanocomposite g–C3N4–MoS2–Ni(OH)2. Morphological investigation using TEM and SEM analyses revealed flower-like structure near fine sheets of Ni(OH)2 and g-C3N4. Fruitfully, the modified surface of the nanocomposite resulted in an enhanced hydrogen storage capability. The hydrogen sorption experiments were carried out at 150 °C for 15 and 30 min intervals under 10 bar hydrogen pressure, and the hydrogen desorption process was carried out from room temperature (RT) to 200 °C with a ramping rate of 15 °C min−1 in an argon medium with a flow rate of 100 mL min−1. During non-isothermal H2 desorption, S150 composite exhibits better hydrogen storage capacity of 2.79 and 3.21 wt% under hydrogenation intervals of 15 and 30 min respectively. Furthermore, S150 desorbed 3.7 wt% H2 in 20 min at isothermal desorption of 200 °C