In Situ Subangstrom‐Thick Organic Engineering Enables Mono‐scale, Ultrasmall ZnO Nanocrystals for a High Initial Coulombic Efficiency, Fully Reversible Conversion, and Cycle‐Stable Li‐Ion Storage.

A solid electrolyte interphase (SEI)‐free surface and fully reversible conversion are simultaneously realized in the Li‐ion storage of a specially designed ZnO porous nanocomposite with in situ surfaces/interfaces organic encapsulation for the first time. The built‐in oxygen‐ and/or moisture‐isolating organic layer of subangstrom thickness not only avoids the SEI formation, but also guarantees monodisperse and ultrasmall dimensions of ZnO nanocrystals, which are crucial for the high initial Coulombic efficiency (ICE) and fully reversible conversion. Benefiting from the high ICE up to 91.4%, stable long‐term cyclibility (95% capacity retention at 1 A g−1 after 1400 cycles), and no sacrificing Li‐ion storage capability (868 mAh g−1 at 0.1 A g−1), the ZnO nanocomposite demonstrates the highest initial Li‐ion utilization efficiency (ILUE, ≈85.4%) among previous transition metal oxide–based full cells. [ABSTRACT FROM AUTHOR]