The conventional method of manufacturing lithium-ion battery electrodes employs a complex slurry casting process with solvents that are not environmentally friendly and process parameters that are often difficult to control. This study explores a solvent-free dry electrode fabrication process of Co- and Ni-free LiMn2O4 (LMO) cathodes using a fibrillated polymer, polytetrafluoroethylene (PTFE). A thick, dry electrode (265–368 μm, 30–64 mg cm–2) of LMO cathode was prepared successfully for the first time. Altering the conductive additives in the LMO dry electrode revealed multiwalled carbon nanotubes (CNTs) as the best conducting agent for dry electrode formulation in terms of conductivity and rate performance. Additionally, an all-dry electrode full cell consisting of both a dry electrode cathode (LMO) and an anode (LTO) delivered a stable cycling performance with a capacity retention of 82.8% after 200 cycles, demonstrating the scope for all-dry electrode full cells for future applications.