Claw‐Inspired Molecular Anchoring for Perovskite Lattice Stabilization

Metal halide perovskites are highly promising for next‐generation photovoltaic devices, but their commercialization is hindered by instability, particularly due to the weakness of undercoordinated A‐site and B‐site cations (e.g., FA + and Pb 2+ ) at lattice edges and grain boundaries. Inspired by the robust gripping mechanism of bird claws, which utilize minimal yet geometrically efficient structures to firmly secure targets, we produce a “molecular claw” strategy at the grain boundaries of the perovskite lattice. This approach introduces a claw‐like molecule capable of multisite anchoring at grain boundaries, effectively stabilizing metastable terminal groups and mitigating failure pathways. Perovskite solar cells employing this strategy achieve exceptional efficiency and stability, with a stabilized efficiency of 24.63% compared to 21.08% for control devices, as well as 1400% increased lifetime of T80 compared to control devices. This claw‐inspired protocol represents a novel example of mechanical structural mimetics applied at the molecular level to anchor active atomic groups, effectively stabilizing the intrinsically unstable soft lattice of perovskites to promote their photovoltaic commercialization process.