In times of climate change and resource scarcity, researchers are aiming to find sustainable alternatives to synthetic polymers for the fabrication of biodegradable, eco-friendly, and, at the same time, high-performance materials. Nanocomposites have the ability to combine several favorable properties of different materials in a single device. Here, we evaluate the suitability of two kinds of inks containing silver nanowires for the fast, facile, and industrial-relevant fabrication of two different types of cellulose-based silver nanowire electrodes via layer-by-layer spray deposition only. The Type I electrode has a layered structure, which is composed of a network of silver nanowires sprayed on top of a cellulose nanofibrils layer, while the Type II electrode consists of a homogeneous mixture of silver nanowires and cellulose nanofibrils. A correlation between the surface structure, conductivity, and transparency of both types of electrodes is established. We use the Haacke figure of merit for transparent electrode materials to demonstrate the favorable influence of cellulose nanofibrils in the spray ink by identifying Type II as the electrode with the lowest sheet resistance (minimum 5 ± 0.04 Ω/sq), while at the same time having a lower surface roughness and shorter fabrication time than Type I. Finally, we prove the mechanical stability of the Type II electrode by bending tests and its long-time stability under ambient conditions. The results demonstrate that the mixed spray ink of silver nanowires and cellulose nanofibrils is perfectly suitable for the fast fabrication of highly conductive organic nanoelectronics on an industrial scale.

Cellulose is a natural polymer with great properties such as high optical transparency and mechanical strength, flexibility, and biodegradability. Hence, cellulose-based foils are suitable for the replacement of synthetic polymers as substrate materials in organic electronics. This article reports the fabrication of ultrathin, free-standing cellulose foils by spraying aqueous 2,2,6,6-tetramethylpiperidine-1-oxyl-nanocellulose (TEMPO) fibrils ink layer-by-layer on a hot substrate using a movable spray nozzle. The resulting foils are only 2 ± 1 µm in thickness with an average basis weight of 1.9 g m−2, which ranges in the same scale as the world's thinnest paper. The suitability of these ultra-thin nanocellulose foils as a sustainable substrate material for organic electronic applications is demonstrated by testing the foils resistance against organic solvents. Furthermore, silver nanowires (AgNWs) and the blend poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) are integrated into the foils, and the foils are molded into 3D paper structures in order to create conductive, paper-based building blocks for organic electronics.