Sulfur removal is significant for fuels used as hydrogen source for modern fuel cell applications and to avoid sulfur poisoning of therein used catalysts. Novel membranes for the polymer-zeolite system with well-defined transport channels are proposed for the sulfur removal. Membranes are fabricated using polyimide (PI) as matrix material and Y zeolites as adsorptive functional materials. By detailed analysis of FT-IR, morphology and adsorption performance of membranes, the process-structure-function relationship is obtained. The results show that the functional zeolites particles are incorporated into three-dimensional channels. For all cases, the inlet fuel can be desulfurized to below 0.1 mg L-1, which means that the outlet fuel can be used as sulfur-free hydrogen source for fuel cell applications. The proposed membranes adsorber may be applied as sulfur trap before the reformer for fuel cells on-board or on-site, and it may be applied in a periodically replaceable form. The desulfurization efforts by membrane are likely to play an influential role for the development of sulfur-free hydrogen source and fuel cell area. Copyright (C) 2013, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.