AbstractManipulating the crystallographic orientation of zinc (Zn) metal to expose more (002) planes is promising to stabilize Zn anodes in aqueous electrolytes. However, there remain challenges involving the non‐epitaxial electrodeposition of highly (002) textured Zn metal and the maintenance of (002) texture under deep cycling conditions. Herein, a novel organic imidazolium cations‐assisted non‐epitaxial electrodeposition strategy to texture electrodeposited Zn metals is developed. Taking the 1‐butyl‐3‐methylimidazolium cation (Bmim+) as a paradigm additive, the as‐prepared Zn film ((002)‐Zn) manifests a compact structure and a highly (002) texture without containing (100) signal. Mechanistic studies reveal that Bmim+ featuring oriented adsorption on the Zn‐(002) plane can reduce the growth rate of (002) plane to render the final exposure of (002) texture, and homogenize Zn nucleation and suppress H2 evolution to enable the compact electrodeposition. In addition, the formulated Bmim+‐containing ZnSO4 electrolyte effectively sustains the (002) texture even under deep cycling conditions. Consequently, the combination of (002) texture and Bmim+‐containing electrolyte endows the (002)‐Zn electrode with superior cycling stability over 350 h under 20 mAh cm−2 with 72.6% depth‐of‐discharge, and assures the stable operation of full Zn batteries with both coin‐type and pouch‐type configurations, significantly outperforming the (002)‐Zn and commercial Zn‐based batteries in Bmim+‐free electrolytes.