Photosynthesis‐Inspired Enhancement of Cellulose Bioplastics Using Hemicellulose‐Derived Biodegradable Polyesters

Abstract Plant growth relies on light, performing photosynthesis throughout their entire life cycle from seedlings to maturity. Plant cell wall strength increases continually due to the photosynthesis of polysaccharides like hemicellulose and their entanglement with cellulose fibers. Here, a photosynthesis‐inspired strategy is presented that utilizes light‐induced formation of hemicellulose‐derived degradable polyester within cellulose fibers to create highly reinforced biocomposites. Photo in situ polymerization of diallyl glyoxylate xylose (DAGX), a stable carbohydrate derived from hemicellulose, within cellulose fibers produces a biocomposite with an interwoven degradable polyester/cellulose fiber structure, mimicking the architecture of plant cell walls. The light‐oriented formation of an interpenetrating network structure enables the biocomposite to achieve a tensile strength of ≈43 MPa, surpassing most commercially available degradable and non‐degradable plastics, exceeding that of cellulose fibers by fivefold. The biocomposite shows excellent water resistance at room temperature yet degrades quickly in hot water, enabling easy recycling of undamaged cellulose fibers for papermaking. Cost and life cycle analyses reveal that the biocomposite is more cost‐effective than commercially available biodegradable plastics, along with a reduced environmental footprint. This study may unlock strategies to fabricate low‐carbon bioplastics by leveraging the abundant and diverse natural polysaccharides library.