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Ultra‐lightweight solar cells have attracted enormous attention due to their ultra‐conformability, flexibility, and compatibility with applications including electronic skin or miniaturized electronics for biological applications. With the latest advancements in printing technologies, printing ultrathin electronics is becoming now a reality. This work offers an easy path to fabricate indium tin oxide (ITO)‐free ultra‐lightweight organic solar cells through inkjet‐printing while preserving high efficiencies. A method consisting of the modification of a poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) ink with a methoxysilane‐based cross‐linker (3‐glycidyloxypropyl)trimethoxysilane (GOPS)) is presented to chemically modify the structure of the electrode layer. Combined with plasma and solvent post‐treatments, this approach prevents shunts and ensures precise patterning of solar cells. By using poly(3‐hexylthiophene) along rhodanine‐benzothiadiazole‐coupled indacenodithiophene (P3HT:O‐IDTBR), the power conversion efficiency (PCE) of the fully printed solar cells is boosted up to 4.73% and fill factors approaching 65%. All inkjet‐printed ultrathin solar cells on a 1.7 µm thick biocompatible parylene substrate are fabricated with PCE reaching up to 3.6% and high power‐per‐weight values of 6.3 W g−1. After encapsulation, the cells retain their performance after being exposed for 6 h to aqueous environments such as water, seawater, or phosphate buffered saline, paving the way for their integration in more complex circuits for biological systems. [ABSTRACT FROM AUTHOR]

Novel emerging materials for organic solar cells, such as nonfullerene acceptors, are paving the way for commercialization of organic photovoltaics. Their utilization in unconventional applications, such as conformable and disposable electronics, has turned the focus to inkjet printing as a fabrication method with advantages including low material usage, rapid digital design changes, and high resolution. In this work, the fabrication of efficient nonfullerene acceptor devices through inkjet printing for organic photovoltaic applications is reported for the first time. The engineering of printable poly‐3‐hexylthiophene:rhodanine‐benzothiadiazole‐coupled indacenodithiophene (P3HT:O‐IDTBR) inks is centered on tuning the rheological properties for proper droplet ejection and the selection of solvents, including hydrocarbons, that meet solubility and volatility requirements to avoid common inkjet printing complications like nozzle clogging. The optimization of printing parameters including drop spacing and deposition temperatures results in homogeneous P3HT:O‐IDTBR films with device efficiencies of up to 6.47% for small lab‐scale devices (0.1 cm2), comparable with that of spin‐coating or blade‐coating. A 2 cm2 inkjet‐printed device is also shown to achieve a remarkable efficiency of 6%. To demonstrate their potential usage in customized applications, large‐area devices are fabricated in the shape of a marine turtle with 4.76% efficiency, showcasing the versatility of the inkjet‐printing process for efficient organic photovoltaics. [ABSTRACT FROM AUTHOR]