The increasing global concern over plastic waste and its environmental impact has led to a growing interest in the development of sustainable packaging alternatives. This study focuses on the innovative use of expired dairy products as a potential resource for producing edible packaging materials. Expired milk and yogurt were selected as the primary raw materials due to their protein and carbohydrate content. The extracted casein was combined with various concentrations of chitosan, glycerol, and squid ink, leading to the studied samples. Chitosan was chosen due to its appealing characteristics, including biodegradability, and film-forming properties, and casein was utilized for its superior barrier and film-forming properties, as well as its biodegradability and non-toxic nature. Glycerol was used to further improve the flexibility of the materials. The prepared hydrogels were characterized using various instrumental methods, and the findings reveal that the expired dairy-based edible packaging materials exhibited promising mechanical properties comparable to conventional plastic packaging and improved barrier properties with zero-oxygen permeability of the hydrogel membranes, indicating that these materials have the potential to effectively protect food products from external factors that could compromise quality and shelf life.