AbstractTo improve the packing efficiency in tank scale, hydrides have been compacted into pellet form; however, poor hydrogen permeability through the pellets results in sluggish kinetics. In this work, the hydrogen sorption properties of compacted 2LiBH4single bondMgH2 doped with 30 wt % activated carbon nanofibers (ACNF) are investigated. After doping with ACNF, onset dehydrogenation temperature of compacted 2LiBH4single bondMgH2 decreases from 350 to 300 °C and hydrogen released content enhances from 55 to 87% of the theoretical capacity. The sample containing ACNF releases hydrogen following a two-step mechanism with reversible hydrogen storage capacities up to 4.5 wt % H2 and 41.8 gH2/L, whereas the sample without ACNF shows a single-step decomposition mainly from MgH2 with only 1.8 wt % H2 and 15.4 gH2/L. Significant kinetic improvement observed in the doped system is due to the enhancement of both hydrogen permeability and heat transfer through the pellet.