Nickel oxides exhibit a great potential as hole transport layers for the fabrication of efficient perovskite light-emitting diodes (LEDs) due to their high carrier mobility and good energy band matching with perovskite nanocrystals. In this work, nickel oxides were directly decorated on the CsPbBr3 nanocrystal surface through adsorption and a sequential oxidation treatment. The resulting sample shows a high photoluminescence quantum-yield of 82%. The LED using CsPbBr3 nanocrystals with nickel oxides achieves a high external quantum efficiency (EQE) of up to 16.8% with a low turn-on voltage of 2.8 V, which is much superior to that of the counterpart LED based on pristine CsPbBr3 nanocrystals (EQE = 0.7%, turn-on voltage = 5.6 V). The excellent performance of the nickel oxide decorated CsPbBr3 nanocrystal device could be attributed to the better energy level matching between the decorated nanocrystals and the transport layers of the device and more balanced charge carrier injection. Furthermore, the operational lifetime of the nickel oxide decorated CsPbBr3 nanocrystal device is 40 times longer than that of the pristine CsPbBr3 nanocrystal device.