A new Ru/Pd/Al2O3/PSS layered membrane was fabricated by electroless plating of palladium and ruthenium for hydrogen separation. Pd and Ru were successively deposited on a pretreated PSS substrate using palladium and ruthenium plating baths at 333 and 358 K, respectively. EDX, XRD and XPS results confirmed the successful plating of ruthenium. Surface analysis showed that the palladium and ruthenium layers did not alloy significantly at temperatures of 723, 823 and 923 K over 100 h. The hydrogen permeation performance of the Pd-Ru composite membrane followed Sieverts' law, suggesting that diffusion of atomic hydrogen through the dense metal layer was rate-limiting. The addition of ruthenium had a negligible effect on hydrogen permeability when the Ru weight content was <= 8 wt%. However, when the Ru content was increased to 11 wt%, H-2 permeability decreased by 10 %. The Pd-Ru membrane exhibited good chemical stability and high H-2/N-2 selectivity in long-term permeation testing.