AbstractAqueous zinc batteries possess intrinsic safety and cost-effectiveness, but dendrite growth and side reactions of zinc anodes hinder their practical application. Here, we propose the extended substrate screening strategy for stabilizing zinc anodes and verify its availability (d_substrate: d_Zn(002) = 1: 1→d_substrate: d_Zn(002)=n:1, n = 1, 2). From a series of calculated phyllosilicates satisfying d_substrate ≈ 2d_Zn(002), we select vermiculite, which has the lowest lattice mismatch (0.38%) reported so far, as the model to confirm the effectiveness of “2d_Zn(002)” substrates for zinc anodes protection. Then, we develop a monolayer porous vermiculite through a large-scale and green preparation as a functional coating for zinc electrodes. Unique “planting Zn(002) seeds” mechanism for “2d_Zn(002)” substrates is revealed to induce the oriented growth of zinc deposits. Additionally, the coating effectively inhibits side reactions and promotes zinc ion transport. Consequently, the modified symmetric cells operate stably for over 300 h at a high current density of 50 mA cm⁻². This work extends the substrate screening strategy and advances the understanding of zinc nucleation mechanism, paving the way for realizing high-rate and stable zinc-metal batteries.