Due to its unique optical properties, two-dimensional (2D) organic-inorganic hybrid perovskite attracts wide attention. In this paper, series of 2D perovskites with the formula [(4-FBA)2(MA)n-1PbnI3n + 1] (4-FBA = 4-FC6H4CH2NH3, MA = CH3NH3, n = 1, 2, 3, n represents the number of 2D perovskite inorganic layers) were obtained by controlling the starting material ratios among 4-fluorobenzylamine, methylammonium iodide and lead iodide. The multilayered perovskite structures were formed by slicing the 3D [MAPbI3] with 4-fluorobenzylamine along the specific crystallographic plane. According to the UV−vis absorption, the bandgaps of the multilayered compounds decreased with the increase of inorganic perovskite layers (Eg = 2.23 eV for n = 1; Eg = 2.01 eV for n = 2 and Eg = 1.78 eV for n = 3), thus leading to their potential application in solar cell.