The present study focuses on enhancing the yield of Mg2FeH6 and its hydrogen storage performances through a novel high-pressure compression approach. For which, MgH2 and Fe powders are first mechanically milled in a molar ratio of 2:1 and subsequently compressed to a cylindrical pellet. Due to the compression, the yield of Mg2FeH6 in the compressed 2MgH(2)-Fe pellet (90%) has been increased by 24% as compared to the reference ball-milled powder (66%). The thermodynamic destabilization of Mg2FeH6 in the pelletized sample is observed through measuring the pressure-composition isotherms, resulting in the reduced ab/desorption enthalpy for the pellet sample (-68.34 and 75.61 kJ/mol H-2, respectively). The hydrogen uptake and release kinetics of Mg2FeH6 is remarkably fast, and it can store/release about 5 wt% H in less than 2.5 min at 400 degrees C. The faster hydrogen ab/ desorption kinetics corresponds to the lower activation energies (36 and 95 kJ/mol H-2, respectively). The excellent yield of Mg2FeH6 and its improved hydrogen storage properties for the compressed pellet are primarily attributed to the microstructural modifications upon high-pressure compression, and also the obtained results for Mg2FeH6 ternary hydride are linked to the literature data based on theoretical calculations. (C) 2020 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.