This article reports the hydrogenation properties of a TiFe0.85Cr0.15 alloy prepared by gas atomization on one hand, and vacuum arc-remelting on the other hand for demonstration and reference, respectively. To evidence the excellent potential of ternary alloying combined with gas atomization process for improving the first hydrogen absorption kinetics, both the atomized powders and the reference crushed ingots were exposed to air from 1 h to as long as 10 days. In spite of the resulting surface oxide layer formation, all specimens still absorbed hydrogen partly thanks to the presence of the C14 Laves phase. As expected, the first hydrogenation kinetics decreased with increasing air-exposure time, but atomized powders not only outperformed the reference counterparts but also remained quite competitive despite surface oxidation. The remarkable kinetic enhancement observed was attributed to the formation of an additional Ti2Fe phase, to an increased amount of C14 Laves phase, as well as to a fine microstructure resulting from the rapid cooling rate involved in gas atomization. Even though different absorption behaviors were observed for all samples, the reaction mechanisms derived from solid-gas reaction models were ascribed to interface- and diffusion-controlled 3D processes in the early and subsequent stage of the first hydrogenation, respectively.