Two-dimensional (2D) organic−inorganic halide perovskites (OIHPs) possess enhanced stability and increased carrier lifetime compared with their three-dimensional (3D) counterparts. In this work, we explore the origin of the layer-dependent stability and strong Rashba effect in 2D OIHPs of α-FABX 3 (B= Ge, Sn, and Pb; X = Cl, Br, I, and FA = HC(NH 2 ) 2 + ) using first-principles calculations. By decreasing the layer number of 2D α-FABX 3 perovskites, both the octahedral tilting angle and formation energy are reduced significantly. As a result of octahedral tilting in 2D α-FABX 3 perovskites, a large Rashba spin splitting is observed, with the Rashba parameters in the range of 0.54−1.58 eV•Å. Moreover, few-layer 2D α-FABX 3 perovskites have a widely tunable band gap from 0.99 to 3.03 eV, making them suitable candidates for both high-efficiency single-junction and tandem solar cells.