A [0001]-oriented zinc metal anode enables sustainable zinc batteries. The study demonstrates that optimizing the crystalline orientation of a Zn metal substrate to expose more Zn(0002) planes enhances the reversibility of Zn metal anodes. However, lattice mismatch between the substrate and overgrowth crystals hinders epitaxial sustainability. The researchers discovered that the presence of crystal grains deviating from [0001] orientation in a Zn(0002) metal anode disrupts the epitaxial mechanism. By creating a [0001]-uniaxial oriented Zn metal anode with a single (0002) texture, the lattice mismatch is eliminated, enabling ultra-sustainable homoepitaxial growth. High-angle angular dark-field scanning transmission electron microscopy (HAADF-STEM) revealed that Zn atoms grow layer-by-layer following a “-ABABAB” arrangement on the Zn(0002) plane. This consistent epitaxial behavior suppresses dendrite formation and improves cycling performance, even in Zn||NH4V4O10 pouch cells, with a high capacity of 220 mAh g⁻¹ for over 450 cycles. The insights gained from this work on the [0001]-oriented Zn metal anode and its persistent homoepitaxial mechanism pave the way for other metal electrodes with high reversibility. Zinc dendrite growth poses a major hurdle in the advancement of Zn-metal batteries, leading to reduced Coulombic efficiency and short circuits. To achieve planarized Zn deposition, tailoring the crystalline orientation of Zn metal anodes to expose the closest-packed Zn(0002) planes has attracted substantial research interest. The study shows that the [0001]-oriented Zn metal anode with a single (0002) texture enables ultra-sustainable epitaxial growth and low inner stress, even under high depth of discharge and/or high areal capacity. The Zn(0002) metal anode offers enhanced cycling when assembled with NH4V4O10. The results emphasize the significance of maintaining a single (0002) texture to achieve sustainable homoepitaxy and suppress dendrite in Zn metal electrode. The Zn(0002) metal anode exhibits a remarkable 80% capacity retention over 450 cycles. The study also highlights the importance of maintaining a single crystalline orientation in Zn(0002) metal anodes for sustainable homoepitaxial growth. The Zn(0002) metal anode has significant potential for practical applications to obtain improved performance and longer lifespans. The Zn(0002) metal anode was tested in full cells configuration using a NH4V4O1A [0001]-oriented zinc metal anode enables sustainable zinc batteries. The study demonstrates that optimizing the crystalline orientation of a Zn metal substrate to expose more Zn(0002) planes enhances the reversibility of Zn metal anodes. However, lattice mismatch between the substrate and overgrowth crystals hinders epitaxial sustainability. The researchers discovered that the presence of crystal grains deviating from [0001] orientation in a Zn(0002) metal anode disrupts the epitaxial mechanism. By creating a [0001]-uniaxial oriented Zn metal anode with a single (0002) texture, the lattice mismatch is eliminated, enabling ultra-sustainable homoepitaxial growth. High-angle angular dark-field scanning transmission electron microscopy (HAADF-STEM) revealed that Zn atoms grow layer-by-layer following a “-ABABAB” arrangement on the Zn(0002) plane. This consistent epitaxial behavior suppresses dendrite formation and improves cycling performance, even in Zn||NH4V4O10 pouch cells, with a high capacity of 220 mAh g⁻¹ for over 450 cycles. The insights gained from this work on the [0001]-oriented Zn metal anode and its persistent homoepitaxial mechanism pave the way for other metal electrodes with high reversibility. Zinc dendrite growth poses a major hurdle in the advancement of Zn-metal batteries, leading to reduced Coulombic efficiency and short circuits. To achieve planarized Zn deposition, tailoring the crystalline orientation of Zn metal anodes to expose the closest-packed Zn(0002) planes has attracted substantial research interest. The study shows that the [0001]-oriented Zn metal anode with a single (0002) texture enables ultra-sustainable epitaxial growth and low inner stress, even under high depth of discharge and/or high areal capacity. The Zn(0002) metal anode offers enhanced cycling when assembled with NH4V4O10. The results emphasize the significance of maintaining a single (0002) texture to achieve sustainable homoepitaxy and suppress dendrite in Zn metal electrode. The Zn(0002) metal anode exhibits a remarkable 80% capacity retention over 450 cycles. The study also highlights the importance of maintaining a single crystalline orientation in Zn(0002) metal anodes for sustainable homoepitaxial growth. The Zn(0002) metal anode has significant potential for practical applications to obtain improved performance and longer lifespans. The Zn(0002) metal anode was tested in full cells configuration using a NH4V4O1