This paper describes the improvement of hydrogen sorption capacity and kinetics of MgH2 by addition of high surface area (≈100m2/g) Raney nickel (RN). Herein, we demonstrate that enhanced hydrogen sorption by MgH2 due to RN is not only linked to the catalytic nature of Ni, but also correlates well with the BET surface area for the MgH2–Ni composites. The Raney Ni also tends to form the less stable Mg2NiH4 hydrides, which desorb hydrogen at much higher pressure as compared with that of the MgH2. We have observed a significant improvement in hydrogen sorption capacity and increase in pressure of hydrogen desorption for MgH2 catalyzed by RN.