Defect generation and propagation in thin films, such as separation membranes, can lead to premature or catastrophic failure of devices such as polymer electrolyte membrane fuel cells (PEMFC). It is hypothesized that defects (e.g., air bubbles, pin-holes, and holes) originate during the manufacturing stage, if precise control is not maintained over the coating process, and they propagate during system operation. Experimental and numerical studies were performed to detect and eliminate defects that were induced during slot die coating of high-viscosity (1 to 40 Pa-s), shear-thinning solutions. The effects of fluid properties, geometric parameters and processing conditions on air entrainment and coating windows (limited set of processing conditions for which defect-free coating exists) were studied. When smaller slot gaps and coating gaps were used, relatively small bubbles were entrained in the coated film. The air bubble sizes increased as the viscosity of the coating solution decreased. A semi-empirical model correlating the maximum coating speed to a solution's material properties, geometric parameters and processing conditions was developed. Such a predictive model will enable engineers to determine the maximum coating boundary for shear-thinning and Newtonian solutions within certain constraints. Smaller coating gaps and low-viscosity solutions produced higher coating speeds. The surface tension property of the coating solution provided stability to the coating bead. Therefore, solutions with higher surface tension could be processed at higher coating speeds.