Recent progress of PSCs in efficiency and stability enhancement is addressed to the change of perovskite composition and crystal optimization. By introducing mixed cations and halide to adjust the composition of the organicinorganic hybrid perovskite, the crystal structure of the perovskite can be effectively improved, which ultimately led to the increased stability and efficiency of the PSCs. Compared with the single cation/ halide perovskite (methylammonium halide, formamidinium lead halide, and cesium lead halide), the mixed perovskite not only has higher PCE but also has better heat and humid air stability. [9][10][11][12] For mixed cation/halide perovskites, despite good optoelectronic properties, the mixing of multiple cations and halogens is prone to localized ionic enrichment during preparation, annealing, and operation. At the same time, as the cation and halide ions move in the builtin electric field of the device, local positive and negative ion vacancies are formed. These defects will cause significant hysteresis in the device and ultimately affect the performance of the device. [13][14][15][16][17] A series of studies on both experimental and theoretical methods [13,18,19] have been reported. Constraining Mixed cation/halide perovskites have led to a significant increase in the efficiency and stability of perovskite solar cells. However, mobile ionic defects inevitably exacerbate the photoinduced phase segregation and selfdecomposition of the crystal structure. Herein, ultrathin 2D nanosheets of oxo-functionalized graphene/dodecylamine (oxo-G/DA) are used to solve ion migration in cesium (Cs)-formamidinium (FA)-methylammonium (MA) triple-cation-based perovskites. Based on the superconducting carbon skeleton and functional groups that provide lone pairs of electrons on it, the ultrathin 2D network structure can fit tightly on the crystals and wrap them, isolating them, and thus reducing the migration of ions within the built-in electric field of the perovskite film. As evidence of the formation of sharp crystals with different orientation within the perovskite film, moiré fringes are observed in transmission electron microscopy. Thus, a champion device with a power conversion efficiency (PCE) of 21.1% (the efficiency distribution is 18.8 ± 1.7%) and a remarkable fill factor of 81%, with reduced hysteresis and improved long-term stability, is reported. This work provides a simple method for the improvement of the structural stability of perovskite in solar cells.