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Printed electronic paper identifies its interest in flexible organic electronics and sustainable and clean energy applications because of its straightforward production method, cost‐effectiveness, and positive environmental impact. However, current limitations include restricted material thickness and the use of supporting substrate for printing. Here, 2D and 3D electronic patterned paper are fabricated from direct ink writing (DIW) nanocellulose and PEDOT:PSS‐based materials using syringe deposition and 3D printing. The conductor patterns are integrated in the bulk of the paper, while non‐conductive sections are used as support to form free‐standing paper. The strong interface between the patterns of electronic patterned paper gives mechanical stability for practical handling. The conductive paper‐based electrode has 202 S cm−1 and is capable of handling electric current up to 0.7 A, which can be used for high‐power devices. Printed supercapacitor papers show high specific energy of 4.05 Wh kg−1, specific power of 4615 W kg−1 at 0.06 A g−1, and capacitance retention above 95% after 2000 cycles. The new design structure of electronic patterned papers presents a solution for additive manufacturing of paper‐based composites for supercapacitors, wearable electronics, or sensors for smart packaging. [ABSTRACT FROM AUTHOR]

Ultrathin devices are rapidly developing for skin‐compatible medical applications and wearable electronics. Powering skin‐interfaced electronics requires thin and lightweight energy storage devices, where solution‐processing enables scalable fabrication. To attain such devices, a sequential deposition is employed to achieve all spray‐coated symmetric microsupercapacitors (μSCs) on ultrathin parylene C substrates, where both electrode and gel electrolyte are based on the cheap and abundant biopolymer, cellulose. The optimized spraying procedure allows an overall device thickness of ≈11 µm to be obtained with a 40% active material volume fraction and a resulting volumetric capacitance of 7 F cm−3. Long‐term operation capability (90% of capacitance retention after 104 cycles) and mechanical robustness are achieved (1000 cycles, capacitance retention of 98%) under extreme bending (rolling) conditions. Finite element analysis is utilized to simulate stresses and strains in real‐sized μSCs under different bending conditions. Moreover, an organic electrochromic display is printed and powered with two serially connected μ‐SCs as an example of a wearable, skin‐integrated, fully organic electronic application. [ABSTRACT FROM AUTHOR]