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Lithium metal batteries suffer from short lifespans and low Coulombic efficiency (CE) due to the high reactivity of Li and the poor stability of the solid electrolyte interphase (SEI). Herein, we propose the concept of a pseudo-concentrated electrolyte (PCE) induced by an electron-deficient additive (4-pyridylboronic acid; 4-PBA) to form a robust, LiF-rich SEI, thus addressing the above issues. Molecular dynamics simulations confirm that 4-PBA can increase the coordination number of PF6- anions in the Li+ solvation sheath to achieve pseudo-concentrated LiPF6 in the electrolyte. Moreover, the 4-PBA can scavenge harmful PF5 decomposed from LiPF6 to stabilize the LiF-rich SEI. The resulting robust LiF-rich SEI promotes Li growth along the SEI/Li interface and represses the growth of Li dendrites. Thus, excellent performance is achieved, with a high CE of 97.1% for a Li||Cu cell at 1.0 ​mA ​cm−2, and over 950 cycles at 0.5 ​mA ​cm−2 for Li||Li symmetric cells with 1.0 ​wt% 4-PBA electrolyte. Meanwhile, the resulting stable boron-containing cathode electrolyte interphase enables Li||LiNi0·6Co0·2Mn0·2O2 (NCM622) cells to achieve excellent stability, with a capacity retention of 86.9% after 200 cycles.