In this study, a catalyst composed of zinc, ferrocyanide, and carbon nanotubes (CNTs) was synthesized and used to enhance the methanolysis of sodium borohydride (NaBH4). The structural characteristics of Zn3[Fe(CN)6]2-CNT catalysts were investigated utilizing X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) analyses and transmission electron microscopy (TEM). The catalytic activity was studied by measuring the volume of hydrogen produced versus time. The results demonstrated a hydrogen generation rate of 51,480 mL min−1 g−1 for methanolysis of 250 mg NaBH4 at 298 K using 10 mg of the catalyst. Varying the catalyst weight for the methanolysis reaction of NaBH4 showed a high generation rate when a weight of 10 mg was used. The impact of the catalyst on the methanolysis reaction resulted in a lower activation energy (Ea) compared to other works, which is 24.14 kJ mol−1. Moreover, other activation parameters, namely enthalpy (ΔH) and entropy (ΔS), were calculated to be 21.641 kJ mol−1 and −98.986 J mol−1, respectively. The catalyst reusability study showed the stability of the hydrogen generation rate over four cycles.