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The matching of band gaps between sub‐cells is essential for high‐performance perovskite/organic tandem solar cells. We systematically investigated various combinations of wide‐bandgap perovskite layers (1.73–1.85 eV) and narrow‐bandgap organic active layers (1.34–1.38 eV). By integrating a 1.80 eV perovskite sub‐cell with a 1.34 eV organic sub‐cell, the optimized tandem device achieves a high PCE of 25.47% with enhanced operational stability. More details are discussed in the article by Li et al . on pages 777–785. image