Metallic lithium is deemed as the “Holy Grail” anode in high-energy-density secondary batteries. Uncontrollable lithium dendrite growth and related issues originated from uneven concentration distribution of Li⁺ in the vicinity of the anode, however, induce severe safety concerns and poor cycling efficiency, dragging lithium metal anode out of practical application. Herein we address these issues by using cross-linked lithiophilic amino phosphonic acid resin as the effective host with the ion-transport-enhancement feature. Based on theoretical calculations and multiphysics simulation, it is found that this ion-transport-enhancement feature is capable of facilitating the self-concentration kinetics of Li⁺ and accelerating Li⁺ transfer at the electrolyte/electrode interface, leading to uniform bulk lithium deposition. Experimental results show that the proposed lithium-hosting resin decreases the irreversible lithium capacity and improves lithium utilization (with the Coulombic efficiency (CE) of 98.8% over 130 cycles). Our work demonstrates that inducing the self-concentrating distribution of Li⁺ at the interface can be an effective strategy for improving the interfacial ion concentration gradient and optimizing lithium deposition, which opens a new avenue for the practical development of next-generation lithium metal batteries.