All inorganic perovskite nanocrystals (NCs) of CsPbX3 (X = Cl, Br, I, or their mixture) are regarded as promising candidates for high-performance light-emitting diode (LED) owing to their high photoluminescence (PL) quantum yield (QY) and easy synthetic process. However, CsPbX3 NCs synthesized by the existing methods, where oleic acid (OA) and oleylamine (OLA) are generally used as surface-chelating ligands, suffer from poor stability due to the ligand loss, which drastically deteriorates their PL QY, as well as dispersibility in solvents. Herein, the OA/OLA ligands are replaced with octylphosphonic acid (OPA), which dramatically enhances the CsPbX3 stability. Owing to a strong interaction between OPA and lead atoms, the OPA-capped CsPbX3 (OPA-CsPbX3) NCs not only preserve their high PL QY (amp;gt;90%) but also achieve a high-quality dispersion in solvents after multiple purification processes. Moreover, the organic residue in purified OPA-CsPbBr3 is only similar to 4.6%, which is much lower than similar to 29.7% in OA/OLA-CsPbBr3. Thereby, a uniform and compact OPA-CsPbBr3 film is obtained for LED application. A green LED with a current efficiency of 18.13 cd A(-1), corresponding to an external quantum efficiency of 6.5%, is obtained. Our research provides a path to prepare high-quality perovskite NCs for high-performance optoelectronic devices.