Biological polymers, such as polysaccharides and polypeptides, offer renewable and biodegradable solutions for a more sustainable future. These polymers comprise natural building blocks, such as amino acids and glycans, which ensure their true environmental benefits at the end of their lifecycle. For example, cellulose is a highly sustainable material with many excellent properties, including renewability, biodegradability, and versatility in its functionality. It can be used in various forms, such as textiles, packaging materials, and building insulation. Here, we studied advanced cellulosic materials produced by blending or creating bi-composites with biomanufactured proteins inspired by squid ring teeth (SRT). Biomanufactured proteins can be synthesized in larger quantities, have a controlled production process, be modified to create desirable variants, and their production can be scaled up or down. Specifically, we engineered recombinant SRT proteins to have high electrostatic charge, induce crystallinity, and provide polar hydroxyl groups, which enhances cellulosic materials’ triboelectric response. The triboelectric voltage of blend triacetate and cellulose fibers increased by 72–108% and 49–57%, respectively, with a protein content of 10% wt. Furthermore, coating proteins on cellulosic fibers to create bi-composite fibers is a highly effective method for doubling (200%) the triboelectric performance. This finding has important implications for developing sustainable triboelectric materials and producing advanced materials using biomanufacturing.