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Abstract Achieving efficient and stable blue light‐emitting perovskite nanocrystals is a significant challenge for next‐generation optoelectronic devices. Here, a dual‐ligand surface engineering strategy is reported for quasi‐2D CsPbBr₃nanoplatelets (NPLs) synthesized via ligand‐assisted reprecipitation. By synergistically co‐introducing didodecyldimethylammonium bromide to passivate bromine vacancies and hexylphosphonic acid to bind undercoordinated lead ions, the NPLs achieved a remarkable photoluminescence quantum yield of 93.7% and a narrow full‐width at half‐maximum of 19.27 nm. The enhanced photoluminescence (PL) lifetime (6.35 ns), reduced crystal disorder, slower bleach recovery kinetics, and improved thermal stability suggest that the suppressed non‐radiative pathways and strong exciton confinement (Eb = 141.76 meV) result from effective surface defect passivation and enhanced radiative recombination. Additionally, surface and structural characterizations confirmed the successful dual‐ligand integration and improved crystal integrity. The treated NPLs retained ∼57% PL under 450 min of ultraviolet (UV) light and ∼55% PL under 70% relative humidity, demonstrating strong UV and moisture stability. A prototype white light‐emitting device fabricated by integrating dual‐ligand‐treated NPLs achieves a wide color gamut (121% National Television System Committee, 90.4% ITU‐R Recommendation BT.2020), demonstrating their potential for high‐performance optoelectronics. This approach promotes defect suppression in low‐dimensional perovskites, paving the way for stable and efficient blue emitters. 

Abstract This study presents the Br‐rich in situ synthesis of blue‐emitting 2D CsPbBr₃nanoplatelets (NPLs) with various Br/Pb ratios using ZnBr₂as a Br precursor to enhance Br ion adsorption significantly. This leads to effective passivation of surface defects, particularly Pb−Br bonds, by increasing the positive charge density around Pb atoms, thus creating a stable bonding environment and reducing defect formation. Consequently, the photoluminescence quantum yield (PLQY) improves from 31.15% for a Br/Pb ratio of 2 to 87.2% for a ratio of 6. NPLs with a Br/Pb ratio of 6 also exhibit longer lifetimes (16.69 ns) and slower bleach recovery dynamics, indicating fewer non‐radiative recombination pathways and effective exciton dynamics. Additionally, NPLs with the Br/Pb ratio of 6 demonstrated better thermal stability, with an activation energy of 124.3 meV, indicating stronger exciton binding. These NPLs also exhibited enhanced stability, with UV tolerance at 43.9% and water resistance at 23.8%, making them suitable for displays and lighting. Furthermore, Br‐passivated CsPbBr₃NPLs are used as blue emitters in prototype white LEDs, achieving a wide color gamut, 126.6% of the National Television Standards Committee and 94.5% of Rec. 2020, demonstrating their potential for high‐quality lighting and advanced display technologies.