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Organic Photovoltaics In article number 2201614, Shuguang Wen, Chunming Yang, Xichang Bao, and co‐workers report a synergistic strategy to fabricate efficient and super flexible thick‐film organic solar cells (OSCs). The proposed comprehensive regulation of intra‐ and inter‐domain interactions in the active layer points to an important research direction for the thickness sensitivity and mechanical stability issues facing flexible OSC applications.