Metal halide perovskite nanocrystals (PeNCs) are emerging as one of the most promising materials for optoelectrical devices such as light‐emitting diode (LED) owing to their tunable band gaps, high color purity, and tolerance to defects. Nevertheless, the materials have not yet demonstrated their full potential in practical applications due to the poor stability of PeNCs and their unsatisfactory performance in devices. In this research, LED devices based on CsPbBr3 NCs are successfully demonstrated as an active light‐emitting layer with enhanced efficiency via potassium doping. The study of the effect of potassium dopant on physicochemical properties of inorganic CsPbBr3 PeNCs shows that potassium cations (K+) remain in the crystal structure of perovskite compound as interstitial defects, which results in better coverage of surface ligands on the PeNCs and improved energy band alignment with adjacent electron injection layer (2,2′,2′‐(1,3,5‐benzinetriyl)‐tris(1‐phenyl‐1‐H‐benzimidazole)) and hole injection layer (poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate) in an LED. As a consequence, the green LED with the K‐doped CsPbBr3 PeNCs shows luminance up to 5759 cd m‐2 and external quantum efficiency (EQE) of 5.6%, which is superior to the pristine device without K‐doping (luminance: 4579 cd m‐2, EQE: 4.8%).