HighlightsThe nucleation overpotential was regulated by sodium L-tartrate to drive smaller critical size of Zn nucleus and accelerate the nucleation rate.The L-tartrate anions and sodium ions can increase de-solvation energy barrier suitably and hinder the agglomerative Zn deposition resepectively.Nucleation overpotential in modified electrolyte could increase from 28.3 to 45.9 mV, and high Zn utilization rate of 80% at current density of 10 mA cm−2can be achieved.Supplementary InformationThe online version contains supplementary material available at 10.1007/s40820-023-01136-z.