A hydrogen-selective nano-composite ceramic membrane was prepared by depositing a dense layer composed of SiO2 and Al2O3 on top of a graded multilayer substrate using co-current chemical vapor deposition (CVD) method. The multilayer substrate was made by dip-coating a macroporous a-alumina tubular support by a series of boehmite solutions to get a graded structure. Using DLS analysis, it was concluded that decreasing hydrolysis time and increasing acid concentration lead to smaller particle size of boehmite sols. XRD analysis was carried out to investigate the structure of intermediate layer and an optimized calcination temperature of 973 K was obtained. SEM images indicated the formation of a graded membrane with a porous intermediate layer having a thickness of about 2 mu m and a dense top selective layer with a thickness of 80-100 nm. Permeation tests showed that H-2 permeance flux decreased from 5 x 10(-5) mol m(-2) s(-1) Pa-1 for a fresh substrate to 6.30 x 10(-7) mol m(-2) s(-1) Pa-1 after 6 h of deposition, but H-2 selectivity over N-2 increased considerably from 5.6 to 203. Copyright (C) 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.