It is highly desirable to design enzyme‐free nanoarray architecture as an efficient three‐dimensional (3D) catalyst electrode for sensitive and selective detection of glucose. In this communication, we report that in situ electrochemical development of an amorphous cobalt‐borate nanoarray supported on carbon cloth (Co–Bi /CC) as a durable and efficient 3D nanoarray electrocatalyst for glucose detection. As a glucose sensor, Co−Bi/CC electrode shows a fast amperometric response toward glucose, a detection limit of 0.042 μM (S/N=3), a response sensitivity of 4191.7 μA mM−1 cm−2. Importantly, it also demonstrates favourable reproducibility and long‐term stability.