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Ultra‐thin stainless‐steel substrates with excellent water‐oxygen barrier properties and high thermal and electrical conductivities are suitable for the fabrication of lightweight and flexible perovskite solar cells (FPSCs). However, the deposition of dense perovskite films on stainless steel by the solution method is crucial because short circuits caused by perovskite holes are fatal to parallel structures. Herein, a single crystal (SC) is incorporated into the precursor solution to reduce the formation of holes in perovskite films on smooth stainless‐steel substrates. Additionally, a magnetic method is developed based on the properties of stainless steel to fix and fabricate FPSCs nondestructively on ultra‐thin stainless‐steel films with a thickness as low as 5 μm. Furthermore, 4,6‐dimethyl‐2‐mercaptopyrimidine (DMI) was introduced to passivate the surface of the perovskite film, optimizing the contact properties of the perovskite heterojunction and adjusting the energy level of the perovskite/C60 interface. Finally, ultra‐thin FPSCs achieved a champion power conversion efficiency (PCE) of 20.24% on an active area of 1.012 cm2 and a power‐to‐weight ratio over 3000 W kg−1. Moreover, under continuous illumination, the stainless‐steel substrates exhibited better photothermal stability than the polymer substrates. This method provides a basis for the fabrication of lightweight, low‐cost, and large‐area FPSCs. [ABSTRACT FROM AUTHOR]