In order to enhance safety, increase energy density, and extend the lifetime of energy storage systems in electric vehicles and renewable energy systems, all-solid-state batteries (ASSBs) have emerged as a promising solution to address the current risks and limitations in lithium-ion batteries (LIBs). However, it has been shown that it is not trivial to achieve ASSBs with adequate cell performance; there are still many challenges present at materials, electrode, and cell levels that need to be addressed. For instance, at materials level low ionic conductivity of the solid electrolytes (SE), insufficient interface contacts as well as electrochemical instability between the active material and the SE in composite cathode (CC) have to be improved. At the electrode and cell level, the manufacturing process limitations such as air and humidity sensitivity of sulfide SEs, residual porosity in the CC, strain/stress during pressing or cycling which lead to delamination and/or crack formation, insufficient/blocked ionic and electronic charge transport pathways have to be overcome. To tackle abovementioned challenges and also to generate a deeper understanding of performance and processability, it is crucial to investigate the relationship between microstructural and electrochemical properties at the particle, interface and electrode level. The aim of this study is to develop a workflow combining high-resolution X-ray microscopy with correlative fs-Laser/FIB preparation and analysis while keeping the air and humidity sensitive sample material under inert conditions. X-ray microscopy is used to determine the homogeneity of the CC thickness as well as occurring cracks and delamination in cathode and separator and to locate areas of interest for further investigation. The feature size ranges from 10 – 500 µm while a large volume can be investigated. The addition of location specific fs-Laser/FIB/SEM, based on the volumetric data, allows for smaller features like the phase distribution, the particle size and distribution as well as microporosity in the CC in the range of <1 – 10 µm can to be investigated. Complementary EDS analysis and 3D-FIB tomography further gives insight into the active surface area at the interface as well as possible reaction products during processing and cycling. This synergetic workflow allows a more comprehensive understanding of the ASSB microstructure over a multitude of length scales.