The effects of NiFe 2 O 4 nanoparticles addition on the dehydrogenation behavior of LiAlH 4 were investigated. The onset dehydrogenation temperature for LiAlH 4 +3 mol % NiFe 2 O 4 sample is 61°C, which decreased by 94°C compared with the as-received LiAlH 4 and released ∼7.2 wt % hydrogen when heated to 180°C. Isothermal desorption measurements show that the 3 mol % NiFe 2 O 4 -doped sample releases ∼7.0 wt % of hydrogen in 91 min at 120°C, which is 6.3 wt % higher than the as-received LiAlH 4 under the same conditions. Through calculating the apparent activation energy of the LiAlH 4 samples with and without NiFe 2 O 4 for the first two dehydrogenation stages, the E a of the LiAlH 4 +3 mol % NiFe 2 O 4 sample is 54.3 and 70.8 kJ/mol, resulting in 52.5 and 59% decrease, respectively, compared with the as-received LiAlH 4 . Analyzing the X-ray diffraction and Fourier transform infrared spectroscopy results, it is reasonable to believe that the remarkable improvement of dehydrogenation properties of NiFe 2 O 4 -doped LiAlH 4 results from the in situ formed LiFeO 2 and Al−Ni compounds, providing the active sites for nucleation and growth of the dehydrogenation products.