Metal-halide perovskite-based green and red light-emitting diodes (LEDs) have witnessed a rapid development because of their facile synthesis and processability; however, the blue-band emission is constrained by their unstable chemical properties and poorly conducting emitting layers. Here, we show a trioctylphosphine oxide (TOPO)-mediated one-step approach to realize bright deep-blue luminescent FAPbBr3 nanoplatelets (NPLs) with enhanced stability and charge transport. The concentration of NPL surface ligands is shown to be progressively tuned via varying the amount of intermediate TOPO due to the acid-base equilibrium between protic acid and TOPO. By effectively optimizing the concentration of surface ligands, the structural integrity of NPL solids can be preserved in ambient air for a week, mainly because of the highly ordered and dense solid assembly and the reduced defects. The removal of excess organic ligands also enables the improvement of charge mobility by orders of magnitude. Ultimately, ultrapure deep-blue perovskite LEDs (439 nm) with a narrow emission width of 14 nm and a peak EQE of 0.14% are achieved at low driving voltage. Our finding expands the current understanding of surface ligand modulation in the development of pure bromide deep-blue perovskite optoelectronics.