Hydrogen generation via the hydrolysis of sodium tetrahydridoborate (NaBH₄) is attractive for in situ-demand applications that require hydrogen gas as an energy source or as a reducing agent. Herein, sulfuric acid-assisted carbonization of Zr-based metal–organic frameworks (MOFs) produced a solid acid zirconium oxo sulfate/carbon (ZrOSO₄/C). X-ray diffraction, high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscopy/mapping, nitrogen gas adsorption–desorption isotherm, and X-ray photoelectron spectroscopy were used to characterize the material’s phase purity and porosity. Data analysis confirmed the porosity and crystallinity of ZrOSO₄/C. The materials catalyzed the hydrolysis process of NaBH₄, producing a high hydrogen generation rate. The acidity of ZrOSO₄/C plays a vital role in the material’s catalytic performance. These observations may open a gateway for new exploration toward designing an effective catalyst for the release of hydrogen gas using hydrides.