New results are reported suggesting that with appropriate levels of Fe doping Mg can rapidly and reversibly absorb up to 7 mass fraction (%) hydrogen at moderate temperatures and pressures useful for hydrogen storage applications. Hydrogenation kinetics and thermodynamics of Mg-4Fe at.% (+/- 1 at.%) thin films capped with Pd at temperatures ranging from 363 K to 423 K were studied by a number of different methods: in situ infrared imaging, volumetric pressure-composition isotherm (PCI) measurements, and ex situ X-ray diffraction and transmission electron microscopy. The hydride growth rate was determined by utilizing wedge-shaped films and infrared imaging; assuming formation of a continuous hydride layer, the growth rate was found to range from approximate to 3.8 nm/s at lower temperature to approximate to 36.7 nm/s at higher temperature. The apparent activation energy of the thermally activated hydrogenation kinetics was measured to be 56 kJ/mol; this value suggests that at low temperatures hydrogen diffusion along grain boundaries of MgH(2) is the mechanism controlling the hydride layer growth. Reproducible PCI measurements of 600 nm-thick uniform films showed a pressure plateau and large hysteresis; from these measurements enthalpy and entropy were estimated as 66.9 kJ/mol and 0.102 kJ/(mol*K), respectively, which are both slightly less than values for pure magnesium (as either films or bulk). The extremely rapid and cyclable kinetics of Mg-4 at.% Fe films suggest that properly grown Mg Fe powders of 1-2 mu m size can be fully charged with hydrogen within 1 mm at temperature near 150 degrees C (423 K), with possible practical hydrogen storage applications. Copyright 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.