The study explores the optimization of crystalline orientation of a Zn metal substrate to enhance the sustainability and reversibility of Zn metal anodes in batteries. By focusing on the [0001]-oriented Zn(0002) texture, the researchers found that lattice mismatch between the substrate and overgrowth crystals was a significant barrier to epitaxial growth. They demonstrated that electrodeposited [0001]-uniaxially oriented Zn metal anodes with a single (0002) texture effectively eliminate lattice mismatch and achieve ultra-sustainable homoepitaxial growth. High-angle angular dark-field scanning transmission electron microscopy revealed that Zn atoms grow layer-by-layer following a "ABABAB" sequence on the Zn(0002) surface. This consistent epitaxial behavior suppresses dendrite formation and improves cycling performance, even in pouch cells with a high capacity of 220 mAh g-1 over 450 cycles. The findings highlight the importance of maintaining a single (0002) texture to achieve sustainable homoepitaxy and suppress dendrite formation in Zn metal electrodes, paving the way for more efficient and stable zinc batteries.The study explores the optimization of crystalline orientation of a Zn metal substrate to enhance the sustainability and reversibility of Zn metal anodes in batteries. By focusing on the [0001]-oriented Zn(0002) texture, the researchers found that lattice mismatch between the substrate and overgrowth crystals was a significant barrier to epitaxial growth. They demonstrated that electrodeposited [0001]-uniaxially oriented Zn metal anodes with a single (0002) texture effectively eliminate lattice mismatch and achieve ultra-sustainable homoepitaxial growth. High-angle angular dark-field scanning transmission electron microscopy revealed that Zn atoms grow layer-by-layer following a "ABABAB" sequence on the Zn(0002) surface. This consistent epitaxial behavior suppresses dendrite formation and improves cycling performance, even in pouch cells with a high capacity of 220 mAh g-1 over 450 cycles. The findings highlight the importance of maintaining a single (0002) texture to achieve sustainable homoepitaxy and suppress dendrite formation in Zn metal electrodes, paving the way for more efficient and stable zinc batteries.