Nanostructured pure Pd and Pd-Fe alloy films for hydrogen separation and membrane reaction were created by pulsed electrodeposition. Short pulse durations, long times between pulses, and a plating temperature of 60 degrees C were found to produce nanostructured crack-free films. Films with Fe content greater than 20 atom % were stable against grain growth to 400 degrees C, and all of the Pd-Fe films synthesized did not experience the alpha-->beta phase transition. The Pd-Fe nano-alloys had very fast hydrogen absorption kinetics at room temperature, without the need for activation.