The synergetic effects of nitrogen and oxygen impurities on the micro-area chemical composition, microstructure, and hydrogen storage performance of V-Ti-Cr-Fe alloys were investigated through X-ray diffraction, scanning electron microscopy, optical microscopy, and pressure-composition-temperature (PCT) analyses. Results show that the hydrogen storage capacity of V₄₀Ti₂₆Cr₂₆Fe₈ alloy is obviously decreased with increasing the nitrogen and oxygen impurities. The mechanism for the decrease is as follows: the oxygen dissolved in V-based alloys suppresses the formation of the dihydride phase, resulting in the decrease in hydrogen capacity (primary effect); while the nitrogen is bound with titanium forming a new nitrogen-titanium-enriched phase, which results in composition change of the main phase and decreases the lattice parameter (secondary effect).