A nano-Zn2SnO4 (ZTO)/cellulose acetate (CA) hybrid coating (CZ) was designed for Zn anodes via a DFT-guided synthesis. DFT calculations revealed ZTO's Zn2+-selectivity and low migration barriers, enabling dual ion-sieving and acceleration effects. The C═O groups in CA formed Lewis acid-base pairs with desolvated Zn2+ and ZTO, synergistically regulating ion flux. The CZ coating combined superior film-forming ability with high Zn affinity, suppressing side reactions while homogenizing Zn2+ deposition. As a result, CZ-Zn anodes achieved stable cycling for 3000 h at 5 mA cm-2. Full cells paired with NH4V4O10 cathodes exhibited extended cyclability and enhanced rate performance. This work provides a universal strategy for Zn anode protection through multifunctional hybrid coatings.