Direct use of metals as battery anodes could significantly boost the energy density, but suffers from limited cycling. To make the batteries more sustainable, one strategy is mitigating the propensity for metals to form random morphology during plating through orientation regulation, e.g., hexagonal Zn platelets locked horizontally by epitaxial electrodeposition or vertically aligned through Zn/electrolyte interface modulation. Current strategies center around obtaining (002) faceted deposition due to its minimum surface energy. Here, benefiting from the capability of preparing a library of faceted monocrystalline Zn anodes and controlling the orientation of Zn platelet deposits, we challenge this conventional belief. We show that while monocrystalline (002) faceted Zn electrode with horizontal epitaxy indeed promises the highest critical current density, the (100) faceted electrode with vertically aligned deposits is the most important one in suppressing Zn metal corrosion and promising the best reversibility. Such uniqueness results from the lowest electrochemical surface area of (100) faceted electrode, which intrinsically builds upon the surface atom diffusion barrier and the orientation of the pallets. These new findings based on monocrystalline anodes advance the fundamental understanding of electrodeposition process for sustainable metal batteries and provide a paradigm to explore the processing–structure–property relationships of metal electrodes. For next-generation batteries, metals-including lithium (Li), sodium (Na), potassium (K), magnesium (Mg), calcium (Ca), zinc (Zn), and aluminum (Al)-have been proposed as anode candidates owing to their high energy density ( 1– 10). To be used as rechargeable battery electrodes, the metal anodes have to be plated and stripped over hundreds of cycles reversibly ( 11, 12). However, the propensity of metal anodes to form random morphology during plating speeds up the capacity fading and internal short-circuit, presenting a fundamental barrier to achieve high reversibility ( 13). The Zn anode is of great interest for its sustainability, low toxicity, and intrinsic safety in aqueous batteries ( 14). More importantly, Zn electrodeposits are typically in the form of hexagonal platelets exposing the minimum surface energy Zn(002) facet due to the hexagonal close-packed (HCP) crystallographic anisotropy ( SI Appendix, Fig. S1) ( 15), which can be used as a model system to study the regulation of electrodeposit morphology evolution.