One of the most important concerns now governing international attention is energy generation. In this work, Ce(NDC)MOF@Bentonite nanocomposite was synthesized and used as a novel and effective catalyst for the green synthesis of hydrogen. The synthesized composite was characterized using X-ray diffraction (XRD), thermogravimetric analysis (TGA), N2-adsorption, Fourier- transform infrared (FT-IR), and scanning electron microscope (SEM) techniques. On the view of the characterized data, a pure and distinct crystalline phase with a highly specific surface area (SBET) of 58.5 m2/g was formed. Moreover, the morphology of the nanocomposite was monitored through scanning (SEM). SEM image which revealed a highly porous surface texture with some large particles with highly spherical morphology. The catalytic performance of the fabricated catalysts was propped via the hydrolysis of sodium borohydride. The effect of NaBH4 concentration, weight of the catalyst, and the reaction temperature on NaBH4 hydrolysis was investigated. The hydrogen generation rate HGR of 116.02 mL min−1g− 1 at 30 °C was achieved using 16 mg of the catalyst and 0.05 M NaBH4. Kinetic and thermodynamic functions including activation energy, enthalpy, entropy, and free energy changed were also estimated. This work suggests that such novel and highly active catalysts hold strong potential as advanced materials for hydrogen energy applications.