A scalable and accessible photoactive formulation with a low synthetic complexity (SC) index is utilized in organic photovoltaic (OPV) fabrication. The formulation readily dissolves in nonchlorinated solvents, and the corresponding photoactive films can be processed by various coating methods to fabricate devices with power conversion efficiencies (PCEs) of 16.1% and 15.2% when using vacuum‐based molybdenum oxide and solution‐processable conducting polymer as the hole transporting layer in the inverted structure, respectively. This prepared device shows superior stability under light exposure. The PCE is maintained 94% of the initial values after 1080 h of light soaking at 100 mW cm−2. Furthermore, the figure of merit based on the ratio of the SC index and PCE indicates the benefit of this formulation for OPV manufacturing, showing the feasibility of commercialization. Eventually, a PCE of 10.3% is demonstrated for a mini‐module fabricated under ambient conditions, with an active area of 32.6 cm2. To our knowledge, this PCE is one of the largest values reported to date for a green solvent and an all‐solution‐processed OPV module with an inverted architecture.

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Solution‐processable hole‐transporting materials are demonstrated to improve the performance of nonfullerene‐based organic photovoltaic devices in an inverted structure. A vanadium oxide (VOX) precursor, used as a sol–gel, is mixed with commercial poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) to form a well‐dispersed VOX:PEDOT:PSS solution. The work function and molecular distribution of the VOX:PEDOT:PSS thin film are examined by ultraviolet photoelectron spectroscopy (UPS) and time‐of‐flight secondary ion mass spectrometry (ToF‐SIMS), respectively. Unlike conventional PEDOT:PSS, VOX:PEDOT:PSS not only is compatible with highly hydrophobic photoactive layers but also aligns well with the highest occupied molecular orbital (HOMO) level of the polymer donor, reaching a power conversion efficiency of 10% (≈100% boost) and achieving an excellent device stability.

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A phosphomolybdic acid (PMA)‐doped poly(3,4‐ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) hole transporting layer (HTL) is developed to effectively optimize the anode interface of inverted organic photovoltaic (OPV) devices. Since a deep‐lying work function of HTL is in favor of reducing the interfacial barrier for hole transporting, superior power conversion efficiencies (PCE) of 9.22% and 10.8% are achieved in fullerene‐based and nonfullerene‐based devices in inverted architecture. Thus‐prepared OPV devices also exhibit excellent photostability and retain 85% of the initial PCE after 1000 h of irradiation under 100 mW cm−2 irradiation. The overall result suggests the practicability and mitigation of efficiency loss when replacing the conventional PEDOT:PSS with PMA‐doped PEDOT:PSS as HTL to fabricate highly efficient, inverted OPV devices.