Unlike organic–inorganic hybrid perovskites, all-inorganic cesium lead halide perovskites hold great promise for developing high-performance optoelectronic devices, owing to their improved stability. Herein, we investigate the perovskite-related CsPb2Br5 nanoplatelets (NPLs) with tunable emission wavelengths via changing the reaction temperatures to 100°C, 120°C, and 140°C. Reaction temperature plays a key role in determining the shapes and thicknesses of the resulting CsPb2Br5 NPLs. A higher temperature is in favor of the formation of smaller and thicker NPLs. To develop their potential applications in optoelectronic devices, green light emitting diodes (LEDs) and photodetectors based on CsPb2Br5 NPLs are fabricated. The green LEDs based on CsPb2Br5 NPLs synthesized at 140°C exhibit an excellent pure green emission (full width at half-maximum of <20 nm) and display a luminous efficiency of 34.49 lm/W under an operation current of 10 mA. Moreover, the photodetector based on CsPb2Br5 NPLs synthesized at 100°C has better performance with a rise time of 0.426 s, a decay time of 0.422 s, and a ratio of the current (with and without irradiation) of 364%.