Halide perovskites have attracted great attention due to their high color purity, high luminance yield, low non-radiative recombination rate, and solution processability. Although the external quantum efficiency of perovskite light-emitting diodes (PeLEDs) is comparable with that of the organic light-emitting diodes (OLEDs) and quantum-dots light-emitting diodes (QLEDs), the brightness is still low compared with the traditional OLEDs and QLEDs. Herein, we demonstrate high brightness and high-efficiency CsPbBr3-based PeLEDs using interface and bulk controlled nanocrystal growth of the perovskite emission layer. The interface engineering by ethanolamine and bulk engineering by polyethylene glycol led to highly crystallized and cubic-shaped perovskite nanocrystals with smooth and compact morphology. As a result, PeLEDs with a high brightness of 64756cd/m2 and an external quantum efficiency of 13.4% have been achieved.