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Magnesium hydride (MgH₂) has received significant attention due to its potential applications as solid-state hydrogen storage media for useful fuel cell applications. Even though MgH₂ possesses several attractive hydrogen storage properties, it cannot be utilized in fuel cell applications due to its high thermal stability and poor hydrogen uptake/release kinetics. High-energy ball milling, and mechanically-induced cold-rolling processes are the most common techniques to introduce severe plastic deformation and lattice imperfection in the Mg/MgH₂. Furthermore, using one or more catalytic agents is considered a practical solution to improve both the de-/rehydrogenation process of MgH₂.These treatments are usually dedicated to enhance its hydrogen storage properties and deduce its thermal stability. However, catalyzation of Mg/MgH₂ powders with a desired catalytic agent using ball milling process has shown some disadvantages due to the uncontrolled distribution of the agent particles in the MgH₂ powder matrix. The present study has been undertaken to employ a cold gas-dynamic spray process for catalyzing the fresh surfaces of mechanically-induced cold-rolled Mg ribbons with Ni powder particles. The starting Mg-rods were firstly heat treated and forged 200 times before cold rolling for 300 passes. The as-treated ribbons were then catalyzed by Ni particles, using cold gas-dynamic spray process. In this catalyzation approach, the Ni particles were carried by a stream of Ar gas via a high-velocity jet at a supersonic velocity. Accordingly, the pelted Ni particles penetrated the Mg-substrate ribbons, and hence created numerous micropores into the Mg, allowed the Ni particles to form a homogeneous network of catalytic active sites in Mg substrate. As the number of coating time increased to three times, the Ni concentration increased (5.28 wt.%), and this led to significant enhancement of the Mg-hydrogen storage capacity, as well as improving the de-/rehydrogenation kinetics. This is evidenced by the high value of hydrogen storage capacity (6.1 wt.% hydrogen) and the fast gas uptake kinetics (5.1 min) under moderate pressure (10 bar) and temperature (200 °C). The fabricated nanocomposite MgH₂/5.28 wt.% Ni strips have shown good dehydrogenation behavior, indicated by their capability to desorb 6.1 wt.% of hydrogen gas within 11 min at 200 °C under 200 mbar of hydrogen pressure. Moreover, this system possessed long cycle-life-time, which extended to 350 h with a minimal degradation in the storage and kinetics behavior.