LAUSR

Two key interfaces in flexible perovskite solar cells (f‐PSCs) are mechanically reinforced simultaneously: one between the electron‐transport layer (ETL) and the 3D metal‐halide perovskite (MHP) thin film using self‐assembled monolayer (SAM), and the other between the 3D‐MHP thin film and the hole‐transport layer (HTL) using an in situ grown low‐dimensional (LD) MHP capping layer. The interfacial mechanical properties are measured and modeled. This rational interface engineering results in the enhancement of not only the mechanical properties of both interfaces but also their optoelectronic properties holistically. As a result, the new class of dual‐interface‐reinforced f‐PSCs has an unprecedented combination of the following three important performance parameters: high power‐conversion efficiency (PCE) of 21.03% (with reduced hysteresis), improved operational stability of 1000 h T90 (duration at 90% initial PCE retained), and enhanced mechanical reliability of 10 000 cycles n88 (number of bending cycles at 88% initial PCE retained). The scientific underpinnings of these synergistic enhancements are elucidated.