Hydrogen storage is a critical step for commercialisation of hydrogen consumed energy production. Among other storage methods, solid state storage of hydrogen attracts much attention and requires extensive research. This study rationally and systematically designs novel solid state hydrides; Li2CaH4 (GHD is obtained as -6.95 wt %) and Li2SrH4 (GHD is obtained as -3.83 wt %) using computational method. As a first step, we suggest and predict crystal structures of solid state Li2CaH4 and Li2SrH4 hydrides and look for synthesizability. Then, the mechanical stabilities of hydrides are identified using elastic constants. Both hydrides fulfil the well-known Born stability criteria, indicating that both Li2CaH4 and Li2SrH4 are mechanically stable materials. Several critical parameters, bulk modulus, shear modulus, Cauchy pressures, anisotropy factors of hydrides and bonding characteristics are obtained and evaluated. Furthermore, electronic and optical band structures of hydrides are computed. Both Li2CaH4 and Li2SrH4 have indirect bands gaps as 96 eV (Gamma-U) and 1.10 eV (Gamma-R). Thus, both materials are electronically semiconducting. Also, Bader charge analysis of hydrides have been carried out. Charge density distribution suggests an ionic-like (or polarized covalent) bonding interaction between the atoms. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.