As a core component, the catalyst layer (CL) is widely used in fuel cell, metal‐air battery, and other energy conversion devices. Herein, a highly efficient method for CL preparation via fast current‐driven synthesis followed by pyrolysis is proposed. Compared with previously reported fabrication procedures of zeolite imidazolate frameworks (ZIF)‐based CLs, this method directly deposits the ZIF precursor onto the conductive substrate in a very short time (≤15 min). The self‐supporting CL, converted from ZIF membrane by simple single‐step pyrolysis, is assembled with the gas diffusion layer to obtain cathode. Electrochemical tests exhibit a small potential gap (0.83 V) between the oxygen reduction and evolution reactions, as well as high performance and excellent stability for Zn‐air battery (241 mW cm–2 at 390 mA cm–2), due to the unique design of a bi‐continuous framework (interconnected pores and long carbon nanotubes) and Co‐based active sites. This work may provide new directions for the fast fabrication of non‐platinum group metal CLs for metal‐air batteries or fuel cell applications.