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Colloidal PbSe nanocrystals (NCs) have gained considerable attention due to their efficient carrier multiplication andemissions across near-infrared and short-wavelength infrared spectral ranges. However, the fast degradation of colloidal PbSe NCs in ambient conditions hampers their widespread applications in infrared optoelectronics. It is well-known that the inorganic thick-shell over core improves the stability of NCs. Here, we present the synthesis of PbSe/PbS core/shell NCs showing wide spectral tunability, in which the molar ratio of lead (Pb) and sulfur (S) precursors, and the concentration of sulfur and PbSe NCs in solvent have a significant effect on the efficient PbS shell growth. The infrared light-emitting diodes (IR-LEDs) fabricated with the PbSe/PbS core/shell NCs exhibit an exteal quantum efficiency (EQE) of 1.3%at 1280 nm. The ligand exchange to optimize the distance between NCs and chloride treatment are important processes for achieving high performance on PbSe/PbS NC-LEDs. Our results provide evidence for the promising potential of PbSe/PbS NCs over the wide range of infrared optoelectronic applications.