Undoped lithiation of stoichiometric spinel using lithium hydride LiH up to the composition Lib>2.25b>Mnb>2b>Ob>4b> was performed. A homogeneous material with a given Li: Mn ratio was obtained by mechanochemical activation with sequential annealing of a LiMnb>2b>Ob>4b>–LiH mixture in a high-purity argon atmosphere and then in air or oxygen at 373–553 K.