Semiconductor nanoplatelets (NPLs) have emerged as a very promising class of colloidal nanocrystals for light-emitting devices owing to their quantum-well-like electronic and optical characteristics. However, their lower photoluminescence quantum yield (PLQY) and limited stability have hampered the realization of their outstanding luminescent properties in device applications. Here, to address these deficiencies, we present a two-step synthetic approach that enables the synthesis of core/shell NPLs with precisely controlled shell composition for engineering their excitonic properties. The proposed CdSe colloidal quantum wells possess a graded shell, which is composed of a CdS buffer layer and a CdZnS gradient layer, and exhibit bright emission (PLQY 75-89%) in the red spectral region (634-648 nm) with a narrow emission line width (21 nm). These enhanced optical properties allowed us to attain low thresholds for amplified spontaneous emission (down to ∼40 μJ/cm) under nanosecond laser excitation. We also studied the electroluminescent performance of these NPLs by fabricating solution-processed light-emitting diodes (LEDs). In comparison to NPL-LEDs with CdSe/CdS core/shell NPLs, which exhibit an external quantum efficiency (EQE) value of only 1.80%, a significantly improved EQE value of 9.92% was obtained using graded-shell NPLs, the highest value for colloidal NPL-based-LEDs. In addition, the low efficiency roll-off characteristics of NPL-LEDs enabled a high brightness of up to ∼46 000 cd/m with an electroluminescence peak centered at 650 nm. These findings demonstrate the paramount role that heterostructure engineering occupies in enhancing the optoelectronic characteristics of semiconductor NPLs toward practically relevant levels.