Leather processing generates a huge amount of chromium (Cr) containing wastes, and one of them is chrome shavings (CS), which frequently end up in landfills. It may be harmful to the environment and human health due to the oxidation of Cr(III) to poisonous Cr(VI). Herein, CS and polyvinyl alcohol (PVA) are used for the preparation of flexible CS-PVA composite sheets, using CS as a skeletal and PVA as a cross-linker by a simple and facile technique. CS-PVA composite sheets are characterized by FT-IR, SEM, STA, and UTM. FT-IR analysis of CS-PVA composite sheets indicated the existence of dominating peaks corresponding to collagen amide bands as well as PVA characteristic bands, and it demonstrates the uniformity of the developed composite sheets. When the amount of PVA is increased, the tensile strength of CS-PVA composite sheets increases from 0.21 to 4.17 N/mm2. With increasing of the amount of PVA, the softness decreases from 6.47 to 3.7 mm, and SEM shows decreasing of pores in the composite sheet. The addition of more PVA makes CS-PVA composite sheets more thermally stable. This facile method of preparing CS-PVA composite sheet is low-cost and eco-friendly, having potential applications in various fields, including clothing, leather goods, decoration, packaging, and footwear products, as well as presenting promising platforms for effective utilization of industrial waste materials.