AbstractOrganic/inorganic hybrid artificial functional layer (AFL) designs of Zn anode have witnessed good progress in stabilizing the Zn anode. However, such processes remain uncapable of simultaneously providing durable protection and fast Zn²⁺migration, especially in high‐rate scenarios. Herein, intrinsic hydrogen‐bond donor (HBD)‐lined organophosphate superionic nanochannels are initially engineered to address this challenge. Due to unique ordered nanochannels with a smaller diameter than that of hydrated Zn²⁺ions and polyanions, hydroxymethyl Zn phosphates (Zn(O₃PCH₂OH, ZnOPC) are first considered for AFL design. The small size can provide an interception for polyanions. Density functional theory calculation indicates that ZnOPC nanochannels possess a 35% lower Zn²⁺migration energy barrier than conventional Zn phosphate, highly consistent with tested results. Additionally, as HBDs, rich ‐CH₂OH groups located at nanochannels impose a targeted hydrogen‐bonding interaction with water molecules. Consequently, at an ultrahigh current density up to 50 mA cm⁻², the Zn@ZnOPC anode shows a 36% lower overpotential than that of the bare Zn anode. As‐assembled Zn @ ZnOPC//NaV₃O₈· 1.5H₂O full cells exhibit an ultralong lifespan of 20 000 cycles at 20 A g⁻¹, with a low capacity‐decay of 0.016% per cycle. This work features a targeted hydrogen bonding‐enhanced desolvation effect occurring in organophosphate superionic nanochannels, which would enlighten to explore reliable fast‐charging aqueous batteries.