We employed roll-to-roll coating in the preparation of 40 μm thick poly[2,2′(m-phenylene)-5,5′bibenzimidazole] (PBI) films for fuel cells using both knife-coating (KC) and slot-die (SD) coating. The films were coated directly from a 9% (w/w) solution of PBI in dimethylacetamide onto a sacrificial low cost paper or plastic based carrier substrate and dried using a hot air oven with a length of 1 m at 140 °C. A web width of 305 mm, a working width of 250 mm and a web speed of 0.2 m min−1 were explored to ensure efficient drying of the thick wet film. A large air flow was found to efficiently avoid skinning. Films were prepared by a single coating step and by two subsequent coating steps in order to explore whether two coating steps gave films with fewer defects. A significant development towards upscaling the PEM fuel cell technology was that the PBI membrane was coated onto a sacrificial carrier substrate allowing for easy recoating on top of the firstly prepared film. It was thus possible to prepare free-standing films by a simple coating procedure followed by delamination from the carrier substrate post-film formation and drying. We finally carried out systematic membrane characterization with respect to solubility, phosphoric acid doping and fuel cell performance. Our results showed that the PBI membranes prepared in this work have identical properties compared to traditionally cast membranes while enabling an increase of a factor of 100 in manufacturing speed.