Polymer electrolyte membrane fuel cells (PEMFCs) and PEM electrolyzer are emerging technologies that produce energy with zero carbon emissions. However, the commercial feasibility of these technologies mostly relies on their efficiency, which is determined by individual parts, including the gas diffusion layer (GDL). GDL transfers fluid and charges while protecting other components form flooding and corrosion. As there is a very limited attention toward the simulation work, in this work, a novel approach was utilized that combines simulation and experimental techniques to optimize the sintering temperature of GDL. Ti64GDL was produced through tape casting, a commercial method famous for producing precise thickness, uniform, and high-quality films and parameters such as slurry composition and rheology, casting parameters, drying, and debinding were optimized. The porosity and mechanical properties of the samples were tested experimentally at various sintering temperatures. The experimental results were compared with the simulated results achieved from the GeoDict simulation tool, showing around 96% accuracy, indicating that employing GeoDict to optimize the properties of Ti64GDL produced via tape casting is a critical step towards the commercial feasibility of PEMFCs and electrolyzer. These findings significantly contribute to the development of sustainable energy solutions.