Aqueous zinc-iodine (Zn-I2) batteries are promising candidates for large-scale energy storage due to the merits of low cost and high safety. However, their commercial application is hindered by Zn corrosion and polyiodide shuttle at I2 cathode. Herein, N,N-bis(2-hydroxyethyl)glycine (BHEG) based interfacial adsorption layers are constructed to stabilize Zn anodes and mitigate polyiodide shuttle according to ion-dipole interactions, by using a strategy of electrolyte additive. The tertiary amine (N(CH2)3) and carboxyl (─COO-) groups in the deprotonated BHEG can reversibly capture H+ and dynamically neutralize OH- ions, efficiently buffering the interfacial pH of Zn metal anodes and suppressing hydrogen evolution reactions. Additionally, the BHEG adsorption layers can repel 39.3% of H2O molecules at the Zn interface, creating a "water-deficient" inner Helmholtz plane and preventing Zn corrosion. Significantly, the N(CH2)3 groups in BHEG also inhibit polyiodide shuttle at the I2 cathode, which exhibits high adsorption energies of -0.88, -0.41, and -0.39 eV for I-, I2, and I3 -, respectively. Attributing to these benefits, the Zn-I2 battery can achieve a high areal capacity of 2.99 mAh cm-2 and an extended cycling life of 2,000 cycles, even at a high mass loading of I2 cathode (≈21.5 mg cm-2).