Disposable paper cups are usually composed of high-grade paper board and an inner polyethylene coatings and are extensively used in daily life. However, most disposable paper cups are only used for a short time and then incinerated or accumulated in landfill at the end of their service due to the difficulty in separating the components, leading to a serious threat to our ecosystem. Therefore, developing a facile and green method to recycle and reuse disposable paper cups is vital. By using ionic liquid 1-allyl-3-methylimidazolium chloride (AmimCl) as a solvent, transparent and homogenous cellulose/polyethylene composite films were successfully prepared from used bamboo-based disposable paper cups through the “one-pot method”, without any pre-treatment. It was found that there was a transformation of cellulose I to II after the dissolution and regeneration processes, and the crystallinity degree of the regenerated cellulose-based materials decreased significantly, resulting in a change in thermal properties. Meanwhile, compared to traditional pure cellulose films, the composite films possessed good UV-shielding properties and hydrophobicity. Moreover, they also displayed good mechanical properties. Additionally, the size of the ground PE coatings displayed obvious effects on the structures and properties of the composite films, where the CPE100 (sieved with 100–200 mesh) possessed the most homogeneous texture and the highest tensile strength (82 Mpa), higher than that of commercial polyethylene film (9–12 MPa), showing superiority as packaging or wrapping materials. Consequently, the goals to fabricate uniform cellulose/polyethylene composite films and valorize the solid waste from disposable paper cups were simultaneously achieved by a facile and green “one-pot method”.