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Efficient and stable wide bandgap (WBG) perovskite solar cells (PSCs) are imperative for fabricating superior tandem devices. However, small crystal grains and light‐induced phase segregation of WBG perovskite result in large open‐circuit voltage (VOC) deficits, critically impeding the development of the related devices. Herein, the effective functional groups of Lewis‐base trans‐Ferulic acid (t‐FA)...