The unique anisotropic properties of colloidal quantum wells (CQWs) make them highly promising as components in nanocrystal-based devices. However, the limited performance of green and blue light-emitting diodes (LEDs) based on CQWs has impeded their practical applications. In this study, alloy CdZnSe core CQWs with precise compositions are tailored via direct cation exchange (CE) from CdSe CQWs with specific size, shape, and crystal structure and utilized hot-injection shell (HIS) growth to synthesize CdZnSe/ZnS core/shell CQWs exhibiting exceptional optoelectronic characteristics. This approach enabled the successful fabrication green and blue LEDs manifesting superior performance compared to previously reported solution-processed CQW-LEDs. The devices demonstrated a remarkable peak external quantum efficiency (20.4% for green and 10.6% for blue), accompanied by a maximum brightness 347,683 cd m for green and 38,063 cd m for blue. The high-performance represents a significant advancement for nanocrystal-based light-emitting diodes (Nc-LEDs) incorporating anisotropic nanocrystals. This work provides a comprehensive synthesis strategy for enhancing the efficiency of Nc-LEDs utilizing anisotropic nanocrystals.