In this work, the hydrogen storage behavior of Ti 2CrV + X wt.% Zr 3Fe, where X = 2, 4, 6, 8 and 10 was investigated. The synthesis of all samples was carried out through arc-melting, followed by comprehensive characterization using X-ray diffraction, scanning electron microscopy, and energy-dispersive spectroscopy. The pure-Ti 2CrV as-cast sample presented a single-phase microstructure. However, the addition of the Zr 3Fe led to a remarkable transformation, resulting in the appearance of a Zr-rich secondary phase. It was found that the first hydrogenation is improved with the addition of at least 6 wt% of Zr 3Fe, avoiding any preheating of the sample. These samples achieved their maximum capacity in approximately 10 min at room temperature. The maximum capacity recorded was 4.2 wt% H for the sample with X = 6 wt% Zr 3Fe, while for X = 8 and 10 wt% Zr 3Fe, the capacity recorded was 4.1 wt% and 4.0 wt%, respectively.