A novel zeolite (HY)-filled polymeric chitosan membrane was prepared. The membrane was characterized by wide-angle X-ray diffraction and a swelling test. The pervaporation (PV) experiments were also performed for an ethanol-water system. The results showed that the crystalline structure of chitosan was damaged with increase in the zeolite content, indicating a strong interaction between the HY zeolite and chitosan. The separation factor of the ethanol-water mixture by PV was improved by the filling zeolite. When the HY zeolite content in the membrane was 20 mass %, the separation factor reached the maximum and remained constant during the PV process.