Green hydrogen (H2) offers a sustainable alternative to non-renewable energy sources. This study focuses on enhancing H2 generation from sodium borohydride (NaBH4) using a platinum nanoparticle (Pt-NP) catalyst supported on a niobium-based coordination compound, [Nb(BDC)0.9(PDC)0.1]n, synthesized via a solvothermal method with 1,4-benzenedicarboxylic acid (BDC) and 2,5-pyridinedicarboxylic acid (PDC). Characterization techniques including Scanning Electron Microscopy (SEM), Energy Dispersive X-ray Spectroscopy (EDS), Brunauer–Emmett–Teller (BET) analysis, Raman spectroscopy, and X-ray diffraction (XRD) confirm the morphology, composition, surface area (398.583 m2g−1), and crystallinity of the material. The in situ synthesized Pt-NPs showed a hydrogen generation rate (HGR) of 86.588 mL min−1 g−1 when alone, while the supported catalyst achieved an enhanced HGR of 119.020 mL min−1 g−1 under optimal conditions (10 mmol% Pt, 0.5 mmol NaBH4, 303.15 K). The low activation energy (Ea) of 16.38 kJ mol−1 indicates efficient catalysis. The catalyst maintained stable performance in recycling tests, demonstrating its potential for practical applications in H2 evolution from NaBH4.