Herein, by using different size of organic molecules as cation templates, we prepared four new two-dimensional (2D) lead halide perovskites, [PrPipz]PbBr 4 (1), [DMEDA]PbBr 4 (2), [TMEDA] 0.5 [DMA]PbCl 4 (3) and [TMA] 4 Pb 3 Cl 10 (4). Under the distinct structural directing effects of organic cations, compounds 1-4 present four different types of 2D inorganic layers. Remarkably, compounds 1, 3 and 4 exhibit broadband blue emissions, while compound 2 exhibits broadband yellow emission upon the excitation of UV light at room temperature. This work paves a way to modulate the crystal structure and photoluminescent property of low-dimensional halide perovskite via structural modulation strategy from the molecular level.