Sulfur removal is significant for fuels used as hydrogen source for fuel cell applications and to avoid sulfur poisoning of therein used catalysts. Novel mixed matrix membranes (MMMs) with well-defined transport channels are proposed for sulfur removal. MMMs are fabricated using polyimide (PI) as matrix material and Y zeolites as adsorptive functional materials. The influence of architecture conditions on the morphology transition from finger-like to sponge-like structure and the "short circuit" effect are investigated. The adsorption and regeneration behavior of MMMs is discussed, combining the detailed analysis of FT-IR, morphology, XPS, XRD and thermal properties of MMMs, the process-structure-function relationship is obtained. The results show that the functional zeolites are incorporated into three-dimensional network and the adsorption capacity of MMMs comes to 8.6 and 9.5 mg S g(-1) for thiophene and dibenzothiophene species, respectively. And the regeneration behavior suggests that the spent membranes can recover about 88% and 96% of the desulfurization capacity by solvent washing and thermal treating regeneration, respectively. The related discussions provide some general suggestions in promoting the novel application of MMMs on the separation of organic-organic mixtures, and a potential alternative for the production of sulfur-free hydrogen source for fuel cell applications. (C) 2012 Elsevier B.V. All rights reserved.