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Lithium's interaction with CsPbBr3 nanocrystals (NCs), can enhancing its intrinsic electrical conductivity (σ) for high‐performance device applications. Herein, two distinctly different modes of Li⁺ interaction with CsPbBr3 NCs: minor lattice insertion (0.07% relative to Cs) and predominant surface passivation is reported through LimPbn alloy formation. In contrast, Li⁺ exhibits significantly reduced interaction with Cs4PbBr6 NCs, which could be due to the persence of lower amount of Pb2+ on the surface of these structures. The σ of CsPbBr3:xLi+ NCs through bottom‐contact devices exhibited a gradual increase from 2.1 × 10−7 to as high as 2.5 × 10−6 S m−1, which is a 50‐fold improvement compared to CsPbBr3 NCs. The enhanced σ is attributed to the presence of Li+ doping and surface passivation of CsPbBr3 by the LimPbn ligated complexes. DFT calculations revealed electron movement from the valence and to conduction band and a reduced bandgap further supporting the inferences from experimental studies. The unique feature of the increased luminescence and σ of CsPbBr3:Li+ NCs is explored for fabricating white light emitting diodes. The luminescence efficacy of the device is in the range of 88.5 to 112.5 lm W−1 which is higher compared to pure CsPbBr3 NCs (96.5 lm W−1), offering a pathway for advanced optoelectronic applications. Lithium doping in CsPbBr3 nanocrystals (NCs) enhances electrical conductivity (50‐fold increase) and photoluminescence quantum yield (50% to 67%) via lattice insertion and LimPbn alloy passivation. Optimized LiBr:PbBr2 ratio enable controlled doping, while hydrolyzed LiBr induces a phase transition to Cs4PbBr6. White LEDs using CsPbBr3:Li+ NCs showed superior luminous efficiency (up to 112.5 lm W−1), advancing optoelectronic applications.

Lithium's interaction with CsPbBr nanocrystals (NCs), can enhancing its intrinsic electrical conductivity (σ) for high-performance device applications. Herein, two distinctly different modes of Li⁺ interaction with CsPbBr NCs: minor lattice insertion (0.07% relative to Cs) and predominant surface passivation is reported through Li Pb alloy formation. In contrast, Li⁺ exhibits significantly reduced interaction with Cs PbBr NCs, which could be due to the persence of lower amount of Pb on the surface of these structures. The σ of CsPbBr :xLi NCs through bottom-contact devices exhibited a gradual increase from 2.1 × 10 to as high as 2.5 × 10 S m , which is a 50-fold improvement compared to CsPbBr NCs. The enhanced σ is attributed to the presence of Li doping and surface passivation of CsPbBr by the Li Pb ligated complexes. DFT calculations revealed electron movement from the valence and to conduction band and a reduced bandgap further supporting the inferences from experimental studies. The unique feature of the increased luminescence and σ of CsPbBr :Li NCs is explored for fabricating white light emitting diodes. The luminescence efficacy of the device is in the range of 88.5 to 112.5 lm W which is higher compared to pure CsPbBr NCs (96.5 lm W ), offering a pathway for advanced optoelectronic applications.