Abstract: The hydrogen barrier property of metallic material is the key factor of hydrogen permeation rate, outgassing rate, and hydrogen embrittlement. It is essential for hydrogen storage, nuclear fusion, accelerator, and other fields. Currently, the mainstream hydrogen barrier method is the coating. Its performance in suppressing hydrogen permeation is considerable. However, the efficiency is low for large-area batch treatment and complex-shaped surface treatment. As a result, it’s necessary to explore more hydrogen barrier techniques. This article uses a high-pressure jet to generate vortex cavitation bubbles. Then, the collapse of the cavitation bubbles generates GPa-level impacts on the surface of the materials. The impacts introduce plastic deformation and residual compressive stress into the surface layer, thus achieving a superficially hardened layer of hydrogen barrier. The results show that the jet vortex cavitation modification reduces hydrogen permeation by 65%, and its hydrogen barrier effect is about 30% better than ball blasting. It has the advantages of green environmental protection, low equipment cost, high processing rate, and good applicability to complex shaped parts. It provides a reliable technical means for hydrogen barrier technology for metal materials.