As the electric vehicle market rapidly expands as an eco-friendly means of transportation, there is a growing demand for innovative manufacturing processes that achieve high energy density while being environmentally sustainable and energy-efficient. To address these challenges, we developed a cathode using a solvent-free electrode process with single-crystalline LiNi0.8Co0.15Al0.05O2 (SCNCA), renowned for its mechanical robustness and high specific capacity. This process involves conformal layers of carbon nanotubes (CNTs) on SCNCA particles, resulting in superior Li+/electronic conductivity along with a cathode active-material ratio of 99.6 wt. %, electrode density of 4.0 g cm−3, and volumetric capacity of 835 mAh cm−3. Furthermore, the 3D digital twin analysis of the dry electrode elucidated the key features responsible for its outstanding electrochemical performance with remarkable clarity. This novel combination of CNT wrapping with solvent-free electrode processing not only increases the energy density but also improves the industrial feasibility of solvent-free electrodes for commercial LIBs application.