Here, we present, for the first time to our knowledge, a comprehensive computational modeling workflow that examines the influence of the degree of calendering on the final performance of slurry-based composite electrodes. This study uses NMC622/Li₆PS₅Cl-based cathode microstructures with the presence of carbon and binder, generated through conventional calendering during manufacturing process simulations. This computational workflow is able to correlate the manufacturing process, the composite cathode microstructure and the cell performance, as it combines Coarse-grained Molecular Dynamics (CGMD) for the manufacturing simulation of the slurry, drying and calendering with a 4D-resolved performance model describing electrochemistry and transport mechanisms. The three-dimensional spatial locations of AM, SE, and Carbon-Binder Domain (CBD) within the electrode, as predicted from CGMD simulations, are considered explicitly as separated phases, each of them with specific physical properties. Our electrochemical performance model permits the study of the impact of the calendering degree on ionic and electronic transport, the heterogeneities of electrochemical reactivity within the electrode volume and its overall electrochemical performance. These findings are intended to provide guidelines for optimizing ASSB composite cathode designs.