Thin films comprising different mass fractions of chitosan/polyethylene oxide (Cs/PEO) were successfully synthesized via ordinary solution casting technique. Synthesized thin films characterized in terms of chitosan content using x-ray diffraction (XRD), Fourier transforms infrared (FT-IR), and scanning electron microscopy (SEM) adopted to study surface morphology. Synthesized membranes exhibit a higher degree of crystallinity, according to XRD data decreases with increasing chitosan content.  Infrared spectroscopy revealed that the studied samples show significant structural changes as a result of intermolecular interactions with the appearance of characteristic peaks belonging to individual polymers. The change in intensity may be attributed to the molecular interaction through strong hydrogen bonds between hydroxyl and amino groups on chitosan molecules and ether groups in PEO. Roughness parameters appear to be correlated with the increase in chitosan content.