In this research, the effects of Zeolite 4 angstrom and ZSM-5 on the separation of C2H6 and C3H8 from CH4 through polyurethane/zeolite mixed matrix membranes (MMM) are evaluated. Physical properties of synthesized polyurethane and polyurethane/zeolite MMM were investigated by FTIR, XRD, TGA and SEM analyses. Results indicate that phase separation of hard and soft segments in polyurethane would be increased by adding butanediamine. (BDA) chain extender in polymer due to the generation of more hydrogen bonds between hard segment domains. The obtained SEM micrographs confirm that the Zeolite is distributed in the polymer matrix homogenously. The results of gas permeation represent that permeability and selectivity of Hydrocarbons are increased by increasing the urea groups in the polymer structure. Moreover, the obtained results of gas permeation of polyurethane-zeolite (4 angstrom) membranes indicate an increase in the permeability of Methane, with the reduction in C2H6/CH4 and C3H8/CH4 selectivity by increasing the Zeolite 4 angstrom up to 10 wt%. In addition, the results of the gas permeation of polyurethane-zeolite (ZSM-5) MMM indicate a significant increment in permeability and selectivity of all Hydrocarbons. The permeability of Propane and its selectivity over Methane is increased from 64.8 Barrer and 2.6 into 117.2 Barter and 3.64 in with 20 wt% filled PU-ZSM 5 MMM, respectively. (C) 2014 Elsevier B.V. All rights reserved.