Abstract Although the photovoltaic performance of perovskite solar cells (PSCs) has reached the commercial standards, the unsatisfactory stability limits their further application. Hydrophobic interface and encapsulation can block the damage of water and oxygen, while the instability induced by intrinsic residual strain remains inevitable. Here, the residual strain in a two‐dimensional (2D) Ruddlesden–Popper (RP) perovskite film is investigated by X‐ray diffraction and atomic force microscopy. It's found that the spacer cations contribute to the residual strain even though they are not in the inorganic cages. Benefited from strain relaxation, the film quality is improved, leading to suppressed recombination, promoted charge transport and enhanced efficiency. More significantly, the strain‐released devices maintain 86?% of the initial efficiency after being kept in air with 85?% relative humidity (RH) for 1080?h, 82?% under maximum power point (MPP) tracking at 50?°C for 804?h and 86?% after continuous heating at 85?°C for 1080?h.
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