Minimization of defects and ion migration in organic–inorganic lead halide perovskite films is desirable for obtaining photovoltaic devices with high power conversion efficiency (PCE) and long‐term stability. However, achieving this target is still a challenge due to the lack of efficient multifunctional passivators. Herein, to address this issue, n‐type goethite (FeOOH) quantum dots (QDs) are introduced into the perovskite light‐absorption layer for achieving efficient and stable perovskite solar cells (PSCs). It is found that the iron, oxygen, and hydroxyl of FeOOH QDs can interact with iodine, lead, and methylamine, respectively. As a result, the crystallization kinetics process can be retarded, thereby resulting in high quality perovskite films with large grain size. Meanwhile, the trap states of perovskite can be effectively passivated via interaction with the under‐coordinated metal (Pb) cations, halide (I) anions on the perovskite crystal surface. Consequently, the PSCs with FeOOH QDs achieve a high efficiency close to 20% with negligible hysteresis. Most strikingly, the long‐term stability of PSCs is significantly enhanced. Furthermore, compared with the CH3NH3PbI3‐based device, a higher PCE of 21.0% is achieved for the device assembled with a Cs0.05FA0.81MA0.14PbBr0.45I2.55 perovskite layer.