Hydrolysis is an efficient way of producing hydrogen by using Mg-based waste. In this study, H₂ production is realized in simulated seawater (i.e., 3.5 wt.% NaCl) using the Elektron21 (EL21) alloy as a reagent. This alloy is a magnesium-based alloy composed of 96 wt.% Mg and 4 wt.% rare earth (approx. 3 wt.% Nd and 1 wt.% Gd). EL21 is known for its excellent corrosion resistance and high tensile strength. The impact of different mechanical treatments (ball milling, cold rolling, cryo rolling, and cryo ball milling) on the hydrolysis yield of the material was discussed. A pretreatment with cryo rolling before ball-milling treatment shows the best hydrolysis performance, with a yield of 90.5% achieved in 10 min in salted water. The ductile-to-brittle transition induced a modification of the microstructure, which explains the good hydrolysis performances.