Environmentally benign and biodegradable chitosan (CS) membranes have disadvantages such as low mechanical strength, high brittleness, poor heat resistance and poor water resistance, which limit their applications. In this paper, home-made cellulose nanocrystals (CNC) were added to CS to prepare CNC/CS composite membranes through mechanical mixing and solution casting approaches. The effects of CNC dispersion patterns and CNC contents on the properties of composite membranes were studied. The analysis of the surface and cross-section morphology of the membranes showed that the dispersion performance of the composite membrane was better in the case that CNC was dissolved in an acetic acid solution and then mixed with chitosan by a homogenizer (Method 2). CNC had a great length-diameter ratio and CNC intensely interacted with CS. The mechanical properties of the composite membrane prepared with Method 2 were better. With a CNC content of 3%, the tensile strength of the composite membrane reached 43.0 MPa, 13.2% higher than that of the CNC-free membrane. The elongation at break was 41.6%, 56.4% higher than that of the CNC-free membrane. Thermogravimetric, contact angle and swelling analysis results showed that the addition of CNC could improve the heat and water resistance of the chitosan membrane.