In this research, the effects of nanocrystallization and incorporation of aluminum, titanium, and carbon nanotubes (CNTs) on hydrogen desorption behavior of Mg2Ni alloy were investigated. Toward this purpose, nanocrystalline Mg2Ni intermetallic compound with average grain size of 20 nm was prepared by ball milling of elemental magnesium and nickel powders. Mg2Ni powder was then ball milled with aluminum and titanium powders for 20 h to dissolve these elements into the Mg2Ni structure, leading to the formation of Mg1.7Al0.15Ti0.15Ni compound. The elemental x-ray mapping analysis revealed the uniform dissolution of aluminum and titanium inside the Mg2Ni structure. Mg2Ni and Mg1.7Al0.15Ti0.15Ni compounds were further ball milled with 3 wt.% CNT for 5 h. The high-resolution field emission scanning electron microscopy and transmission electron microscopy revealed that CNTs have retained their tubular shape after ball-milling process. The hydrogen desorption properties of the samples were identified using a Sieverts-type apparatus at 473 K. The Mg2Ni, Mg2Ni-CNT, and Mg1.7Ti0.15Al0.15-CNT samples showed the desorbed hydrogen of 0.17, 0.25, and 0.28 wt.% after 1 h, respectively, indicating 47 and 65% increase in the hydrogen desorption capability of Mg2Ni via CNT addition and co-presence of aluminum-titanium-CNT. The direct hydrogen diffusion through CNTs and development of local atomic distortion due to substitution of magnesium atoms by aluminum and titanium appears to be responsible for enhancement of desorption behavior of Mg1.7Al0.15Ti0.15-3 wt.% CNT.