Two-dimensional Cs2Pb(SCN)2I2 perovskite has an ultra-small interlayer spacing, inducing a series of interesting semiconductor properties, such as efficient interlayer carrier transport as well as lower exciton binding energy compared to perovskites with long alkylammonium cations. The prepared Cs2Pb(SCN)2I2 photodetector achieves a high on/off ratio of 2.1 × 104 with a specific detectivity of 6.2 × 1011 jones to 450 nm visible light, and a high sensitivity of 2747 μC Gyair-1 cm-2 to X-rays.