The magnesium borohydride – ethylenediamine (en) compound Mg(en)1.2(BH4)2 exhibits high Mg-ion conductivity above room temperature. To study the dynamical properties of this compound and its partially deuterium-substituted counterpart, we have measured the 1H, 2D, and 11B nuclear magnetic resonance (NMR) spectra and spin-lattice relaxation rates over a wide temperature range (6–324 K). Our measurements have revealed a coexistence of four types of BH4 reorientational jump processes with different activation energies. For the fastest of these processes characterized by the activation energy of 47(3) meV, the unusually high reorientational mobility is retained down to low temperatures, so that the corresponding H jump rate is of the order of 108 s−1 near 70 K. The presence of fast reorientational motion of [BH4]− anions in Mg(en)1.2(BH4)2 supports the idea that anion reorientations may facilitate the cation diffusion. In the studied temperature range, we have not found any distinct signs of localized motion of the ethylenediamine molecules or their fragments at the NMR frequency scale. © 2023 Elsevier B.V.