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NaBH₄ is a very cheap and hydrogen-rich material, as well as a potential hydrogen store. However, the high temperature of its thermal decomposition (above 530 °C) renders it inapplicable in practical use. Here, we studied the effect of addition of diverse V-containing catalysts on thermal hydrogen desorption. It turns out that mechanochemical doping of NaBH₄ with vanadium metal, its oxides, or nanoparticles lowers the temperature of pyrolysis significantly. Notably, NaBH₄ milled for 3 h with 25 wt.% V₂O₅ or VO₂ releases ca. 70% of stored hydrogen in the temperature range of ca. 370–450 °C. On the other hand, precursors and solvents used to prepare rather uniform vanadium nanoparticles (~4 nm) suspended in THF or less uniform and larger ones (~15 nm) in o- difluorobenzene have adverse effect on the purity of hydrogen evolved.