The 2‐D nanostructure, due to unprecedented physical, electronic, and chemical properties, was widely dedicated to the zooms of electrocatalysis, batteries, supercapacitors, solar cells, photocatalysis and sensing platforms. Herein, we reported a sort of low‐applied potential non‐enzymatic glucose sensor, which used ultrathin 2‐D CuS nanowall arrays (CuS‐NWAs) fabricated directly onto fluorine‐doped tin oxide glass by potentiostatically deposition approach. Meaningfully, the potentiostatical‐deposition time can control precisely the frame of 2‐D CuS‐NWAs on size and thickness and assist to ferret out the growing mechanization by analyzing the copper valence. Then, CuS‐NWAs‐based non‐enzymatic glucose sensor presented the high sensitivity (2610 μA mM−1 cm−2), a low detection of 17 nM, fast respond time (1.5–6.2 s) and low detection limits (2.6–17.7 nM, S/N=3) regardless of an applied potential as low as 0.33 V (vs. Ag/AgCl), attributed to that the 2‐D CuS‐NWAs offer large active area with numerous exposed active points, a low‐resistance electron‐shuttling passage and door‐opened glucose‐diffusion channel. Additionally, it was found that the sensitivity of CuS‐NWAs‐based non‐enzymatic glucose sensors can be optimized by altering electrodeposition duration for CuS‐NWAs growth. Confirmedly, the 2‐D CuS‐NWAs can be promised as a new system for high‐performance electrochemical sensors with excellent properties of selectivity, stability and reproducibility.