This study deals to synthesize LiBH4 by means of mechano-chemical reaction, in which LiBO2 and MgH2 were utilized. In order to obtain 90% LiBH4 purity, optimum reaction conditions were analyzed at different values of reactant ratio and duration. In addition, commercial LiBH4 was hydrolyzed with CoI2 supported on activated carbon (AC). In order to follow up the intermediate steps of the studies FT-IR, XRD analyses have been used. Activation energy of the dehyrdogeneration reaction was searched at different reaction temperatures and determined as 33.12 kj/mol. As an optimum operation time for ballmilling were recorded as 1000 min and reactant ratio (MgH2/LiBO2) were found as 1.0. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.