Nanocrystal‐based light‐emitting diodes (Nc‐LEDs) have immense potential for next‐generation high‐definition displays and lighting applications. They offer numerous advantages, such as low cost, high luminous efficiency, narrow emission, and long lifetime. However, the external quantum efficiency (EQE) of Nc‐LEDs, typically employing isotropic nanocrystals, has been limited by the out‐coupling factor. Here we demonstrate efficient, bright, and long lifetime red Nc‐LEDs based on anisotropic nanocrystals of colloidal quantum wells (CQWs). Through modification of the substrate's surface properties and control of the interactions among CQWs, we successfully spin‐coated a self‐assembled layer with an exceptionally high distribution of in‐plane transitions dipole moment (TDM) of 95%, resulting in an out‐coupling factor of 37%. Our devices exhibit a remarkable peak external quantum efficiency (EQE) of 26.9%, accompanied by a maximum brightness of 55,754 cd m−2 and a long operational lifetime (T95@100 cd m−2) over 15,000 h. These achievements represent a significant advancement compared to previous studies on Nc‐LEDs incorporating anisotropic nanocrystals. We expect our work to provide a general self‐assembly strategy for enhancing the light extraction efficiency of Nc‐LEDs based on anisotropic nanocrystals.This article is protected by copyright. All rights reserved