Attempts have been made to bring eco-friendly biomaterials into high-end electronic devices that require both high performance and durability. Polysaccharides, glycosidically linked monosaccharide units, are of particular interest because they serve as a promising material, owing to their environmentally friendly and adaptable features. We used a carbonized polysaccharide eco-material encompassing nanoparticles and chitosan to study the carrier-transport behavior of β-glucosic materials. Chitosan composites incorporating nanoparticles were prepared and then carbonized to control the crystal structure of the material. Three kinds of metal-insulator-metal devices were fabricated using carbonized materials, and their carrier-transport properties were analyzed. The results showed that the addition of cellulose nano-whiskers (CNWs) into chitosan leads to a more ordered carbon structure, increasing the charge transport in the carbonized material. We anticipate that carbonizing nanoparticle dispersed green composites provides a new pathway for the development of sustainable and environmentally benign material systems.