Although Li-ion batteries are very promising for energy storage applications, their areal capacity is quite low (2.09 mAh cm-2 for conventional LiFePO4 on aluminum foil). The aim of this work is to enhance the areal capacity of LiFePO4 cathode via Surface-Engineered Tape-Casting (SETC) technique. SETC technique enables fabrication of strong stand-alone structured carbon nanotube (CNT) sheet with tunable thickness and composition. The CNTs form electrically conductive networks that also result in enhancing the charge transport of Li-ions. In addition, areal capacity will be increased by using the following approaches: increasing the thickness of CNT-LiFePO4 sheet and changing the CNT/LiFePO4 ratio. We will determine the optimum thickness and composition of the CNT-LiFePO4 sheet. Batteries will be assembled in a glove box and characterized (CV, charge-discharge, EIS) using a potentiostat/galvanostat. Investigation of the multi-layered CNT-LiFePO4 sheets by scanning electron microscopy, Raman scattering spectroscopy and X-ray diffraction is also in progress. Preliminary results show 0.4 mAh cm-2 for 2 layers of CNT-LiFePO4 (CNT:LiFePO4 = 1:1, w/w ratio). Fabrication of the electrodes with more than 10 layers of CNT-LiFePO4 is in progress. Such thick CNT-LiFePO4 electrodes is very good candidate for applications which is very sensitive to weight but not sensitive to size, such as space applications and electrical vehicles.