Pd60Cu40 wt% (Pd47.3Cu52.7 at%) membranes were surface modified by depositing Pd thin films of three different thicknesses (similar to 100, 800 and 1400 nm) on to one side of a range of as-received Pd60Cu40 wt% cold-rolled foils via magnetron sputtering. The hydrogen permeability of the membranes was then measured and compared to the uncoated material. The Pd65Cu40 wt% membrane coated with a 1400 nm thick Pd thin film positioned on the feed side (445 kPa of hydrogen pressure) during hydrogen permeability measurements and cycled between 50 and 450 degrees C achieved the highest hydrogen permeability of 1.09 x 10(-8) mol m(-1) s(-1) Pa-0.5 at 450 degrees C in the third cycle. This is a 58% increase on the value measured for the as-received Pd60Cu40 wt% membrane under the same conditions. This improvement can be attributed to a Pd-rich Pd-Cu face centred cubic (FCC) phase forming through interdiffusion between the Pd thin film and bulk Pd-Cu membrane as a result of the test conditions used during hydrogen permeability measurements. This introduces a larger hydrogen concentration gradient across the membrane due to the relatively high hydrogen solubility of the Pd-rich Pd-Cu FCC phase resulting in the observed increase in permeability. The Pd60Cu40 wt% membranes coated with a similar to 1400 am and similar to 800 nm thick Pd thin film retained an almost pure Pd surface throughout cycling between 50 and 450 degrees C with a feed and permeate hydrogen pressure of 445 and 100 kPa, respectively. For the deposition technique and test conditions used throughout this work, these surface modified Pd-Cu membranes appear to stabilise the Pd thin films upon cycling across the critical temperature of 295 degrees C. (C) 2015 The Authors. Published by Elsevier B.V.