Zein, a predominant corn protein, is an alcohol-soluble protein extracted from corn and is characterized by unique film-forming properties. The characteristic brittleness of zein diminishes its usefulness as a structural material. The objective of this work was to study the effect of gamma-irradiation on improving the performance of zein films in packaging applications. This goal has been achieved by irradiating zein film-forming solutions with various doses of gamma-rays, namely, 10, 20, 30, and 40 kGy at dose rate of 10.5 kGy/h, using a Co(60) gamma-radiation source. The impact of radiation process on the structural properties has been explored through far-UV CD spectral analysis and scanning electron microscopy. Additionally, viscosity changes that reflect the effect of radiation treatment on degradation and/or cross-linking of protein chains have been measured. However, improvements in the performance of zein films as packaging materials that can be accomplished by radiation treatment have been investigated via monitoring of the color, surface density, roughness, mechanical properties (tensile strength and elongation percentage), water uptake, and water barrier properties. The results indicated that gamma-irradiation treatment of the film-forming solution can be used to improve the water barrier properties, as well as color and appearance of the zein films. Moreover, a sterilization effect is considered to be an additional advantage for applying gamma- irradiation.