Abstract Flexible perovskite solar cells (FPSCs) with high stability in moist air are required for their practical applications. However, the poor mechanical stability under high humidity air remains a critical challenge for flexible perovskite devices. Herein, inspired by the exceptional wet adhesion of mussels via dopamine groups, we propose a multidentate-cross-linking strategy, which combine multibranched structure and adequate dopamine anchor sites in three-dimensional hyperbranched polymer to directly chelate perovskite materials in multiple directions, therefore construct a vertical scaffold across the bulk of perovskite films from the bottom to the top interfaces, intimately bind to the perovskite grains and substrates with a strong adhesion ability, and enhance mechanical durability under high humidity. Consequently, the modified rigid PSCs achieve superior PCE up to 25.92%, while flexible PSCs exhibit a PCE of 24.43% and maintain 94.1% of initial PCE after 10,000 bending cycles with a bending radius of 3 mm under exposed to 65% humidity.