Here, the preparation of transparent amorphous oxide semiconductor (AOS) films with unprecedented conductivity via an optimized activation process under hydrogen atmosphere for applications in solution‐processed large‐area optoelectronics is reported. Owing to their high cost and mechanical vulnerability, conventional vacuum‐processed indium–tin oxide (ITO) electrodes are inappropriate for use in next‐generation flexible and wearable electronic devices and systems. As an alternative to the ITO electrodes, solution‐processed AOS films, such as a‐IZO and a‐ZITO, with an optimized composition and postreduction treatment under hydrogen show the highest electrical conductivity of ≈300 S cm−1 and a high optical transmittance of over 90% at 550 nm. The microstructures and electrical properties of these AOS films are also studied in order to determine the optimized chemical composition and postreduction conditions. It is found that a controlled hydrogen reduction treatment of AOS films is critical for achieving high electrical conductivity by suppressing the surface morphology degradation and grain boundary disconnection. Furthermore, the a‐IZO transparent conductive electrodes are successfully implemented for high efficiency organic photovoltaic cells based on the PTB7/PC71BM active layers. This technique promises the low‐cost fabrication of high mobility and/or conductive AOSs for their applications in large‐area transparent and flexible optoelectronics.