Graded silicalite-1 substrates with a high gas permeability and low surface roughness have been produced by pulsed current processing of a thin coating of a submicron silicalite-1 powder onto a powder body of coarser silicalite-1 crystals. Thin zeolite films have been hydrothermally grown onto the graded silicalite-1 support and the all-zeolite membranes display an excellent CO2/H-2 separation factor of 12 at 0 degrees C and a CO2 permeance of 21.3 x 10(-7) mol m(-2) s(-1) Pa-1 for an equimolar CO2/H-2 feed at 505 kPa and 101 kPa helium sweep gas. Thermal cracking estimates based on calculated surface energies and measured thermal expansion coefficients suggest that all-zeolite membranes with a minimal thermal expansion mismatch between the graded substrate and the zeolite film should remain crack-free during thermal cycling and the critical calcination step. (C) 2015 The Authors. Published by Elsevier B.V.