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In this work, a low cost air-assisted cylindrical liquid jets spraying (ACLJS) system was developed to prepare high-performance catalyst-coated membranes (CCMs) for proton exchange membrane fuel cells (PEMFCs). The catalyst ink was flowed from a cylindrical orifice and was atomized by an air stream fed from a coaxial slit and sprayed directly onto the membrane, which was suctioned to a heated aluminum vacuum plate. The CCM pore architecture including size, distribution and volume can be controlled using various flow parameters, and the impact of spraying conditions on electrode structure and PEMFC performance was investigated. CCMs fabricated in the fiber-type break-up regime by ACLJS achieved very high performance during PEMFC testing, with the top-performing cells having a current density greater than 1900 mA/cm2 at 0.7 V under H2/O2 flows and 700 mA/cm2 under H2/Air at 1.5 bar(absolute) pressure and 60% gas RH, and 80°C cell temperature.