Aiming to advance the technical maturity of CO2 electrolysis to formic acid, various gas diffusion layers (GDLs) are investigated for their suitability as carbon‐based substrate for gas diffusion electrodes (GDEs) and their effect on the electroreduction of CO2 to formate. Particular attention lies on the elucidation for the effect of the GDL thickness, hydrophobic treatment, and presence of a microporous layer (MPL) on the GDE performance in terms of Faradaic efficiency. Based on the investigation it is found that the GDL thickness has no discernible influence on the Faradaic efficiency, while a GDE with a hydrophobic treatment of 10 % PTFE outperforms a GDE based on a GDL with 30 % PTFE. Furthermore, the presence of a MPL is found to be of marked importance to achieve relevant current densities given its effect on the focus of the catalyst layer on the GDE surface after spray coating, the wetting, and the electrical conductivity.