Open-cathode polymer electrolyte membrane fuel cells (PEMFCs) utilize a unique air-cooled system design to eliminate the humidifiers, air compressor, and liquid cooling loop of conventional, liquid-cooled PEMFC systems, thereby greatly reducing system cost. However, the open-cathode PEMFC performance is restricted by poor humidification, high membrane and charge transfer resistances, and overheating due to inefficient thermal and water management. This work aims to strategically modify the membrane electrode assembly (MEA) design to overcome these issues and achieve high open-cathode PEMFC performance that approaches that of liquid-cooled systems. The use of thinner membrane along with short side chain ionomer is found to elevate the cell performance due to increased water retention at the cathode catalyst layer (CCL) and decreased ohmic losses. Thinner gas diffusion layers with high porosity enable additional cell performance increment by improving oxygen availability at the CCL. An overall current density rise of 88% at 0.6 V and 53% at 0.4 V is achieved by the strategically designed MEA for open-cathode cells. The enhanced power density enabled by the custom MEA can both reduce the stack cost and expand the power range of open-cathode PEMFCs, thus expanding their potential use for low-cost fuel cell system applications.