In this study, a new multi-layer hybrid nanocomposite membrane named MFI/GO/ZIF-8 has been synthesized. This membrane combines three nanoporous materials with diferent morphologies in one membrane without using polymer materials. This allows access to a previously accessible region of very high permeability and selectivity properties. In addition to introducing a new and efcient MFI/GO/ZIF-8 membrane in this work, controlling the pore size of the zeolite layer has been investigated to increase the selectivity and permeability of propylene. The membrane was made using a solvent-free hydrothermal method and a layer-by-layer deposition method. To control the pore size of the MFI layer, a two-step synthesis strategy has been implemented. In the frst step, three key parameters, including crystallization time, NaOH concentration and aging time of initial suspension, are controlled. In the second step, the efect of three additional parameters including hydrothermal time, hydrothermal temperature and NH4F concentration has been investigated. The results show that the optimal pore size has decreased from 177.8 nm to 120.53 nm (i.e., 32.2%). The MFI/GO/ZIF-8 membrane with fne-tuned crystal size in the zeolite layer was subjected to detailed tests for propylene selectivity and permeability. The structural characteristics of the membrane were also performed using FT-IR, XRD, FESEM and EDS techniques. The results show that the synergistic interaction between the three layers in the nanocomposite membrane signifcantly improves the selectivity and permeability of propylene. The permeability and selectivity of propylene increased from 50 to 60 GPU and from 136 to 177, respectively, before and after precise crystal size control. MFI/GO/ZIF-8 membrane by controlling the pore size of the zeolite layer shows a signifcant increase of 23.1% in selectivity and 16.7% in propylene permeability compared to the initial state. Also, due to the precise synthesis method, the absence of solvent and the use of cheap support, the prepared membrane is considered an environmentally friendly and low-cost membrane. This study emphasizes the potential of increasing the selectivity and permeability of propylene in the MFI/GO/ZIF-8 hybrid membrane by controlling the crystal size of the zeolite layer
