Lithium-ion battery (LIB) performance is significantly influenced by its manufacturing process. Manufacturing of an optimized electrode can incur high production costs such as high energy consumption, high scrap rates and emissions. This is due to the process that consists of a series of manufacturing steps presenting a complex interrelationship, thus limiting the understanding of performance as a function of manufacturing parameters. While several empirical and computational methods are employed for optimization, they are demanding in terms of resources such as materials or computational effort. By leveraging Deep Learning (DL), we can enhance our understanding of the complex manufacturing processes and accelerate its optimization. We propose a data-driven supervised DL methodology to complement physics-based LIB cathode manufacturing simulations. The trained DL-based predictive model integrates well into the manufacturing simulation framework to forecast cathode slurry microstructures. The DL model demonstrates robust predictive performance for LIB NMC-111 and LiFePO4–based slurries and slurries for a solid-state battery NMC-622/argyrodite composite electrode preparation. While the current work is focused on the cathode slurry process, the proposed methodology has potential for application to drying and calendering steps. This approach will be helpful in streamlining lab-scale electrode manufacturing, and reducing errors, waste and resource consumption.