Slot‐die coating is generally regarded as the most effective large‐scale methodology for the fabrication of organic solar cells (OSCs). However, the corresponding device performance significantly lags behind spin‐coated devices. Herein, the active layer morphology, flexible substrate properties, and the processing temperature are optimized synergistically to obtain high power conversion efficiency (PCE) for both the flexible single cells and the modules. As a result, the 1 cm2 flexible devices produce an excellent PCE of 12.16% as compared to 12.37% for the spin‐coated small‐area (0.04 cm2) rigid devices. Likewise, for modules with an area of 25 cm2, an extraordinary PCE of 10.09% is observed. Hence, efficiency losses associated with the upscaling are significantly reduced by the synergistic optimization. Moreover, after 1000 bending cycles at a bending radius of 10 mm, the flexible devices still produce over 99% of their initial PCE, whereas after being stored for over 6000 h in a glove box, the PCE reaches 103% of its initial value, indicating excellent device flexibility as well as superior shelf stability. These results, thus, are a promising confirmation the great potential for upscaling of large‐area OSCs in the near future.

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