Indiana University-Purdue University Indianapolis (IUPUI) / The prevalent applications of energy storage devices have incited wide-spread efforts on production of thin, flexible, and light-weight lithium-ion batteries. In this work, lithium-ion batteries using novel flexible paper-based current collectors have been developed. The paper-based current collectors were fabricated from carbon nanotube (CNT)-coated wood microfibers (CNT-microfiber paper). This thesis presents the fabrication of the CNT-microfiber paper using wood microfibers, coating electrode materials, design and assemblies of battery, testing methodologies, and experimental results and analyses. Wood microfibers were coated with carbon nanotubes and poly(3,4-ethylenedioxythiophene) (PEDOT) through an electrostatic layer-by-layer nanoassembely process and formed into a sheet, CNT-microfiber paper. The CNT loading of the fabricated paper was measured 10.1 μg/cm2 subsequently considered. Electrode material solutions were spray-coated on the CNT-microfiber paper to produce electrodes for the half and full-cell devices. The CNT current collector consists of a network structure of cellulose microfibers at the micro-scale, with micro-pores filled with the applied conductive electrode materials reducing the overall internal resistance for the cell. A bending test revealed that the paper-based electrodes, compared to metal ones, incurred fewer damages after 20 bends at an angle of 300o. The surface fractures on the paper-based electrodes were shallow and contained than metallic-based electrodes. The micro-pores in CNT-microfiber paper structure provides better adherence to the active material layer to the substrate and inhibits detachment while bending. Half-cells and full-cells using lithium cobalt oxide (LCO), lithium titanium oxide (LTO), and lithium magnesium oxide (LMO) were fabricated and tested. Coin cell assembly and liquid electrolyte was used. The capacities of half-cells were measured 150 mAh/g with LCO, 158 mAh/g with LTO, and 130 mAh/g with LMO. The capacity of the LTO/LCO full-cell also was measured 126 mAh/g at C/5 rate. The columbic efficiency of the LTO/LCO full-cell was measured 84% for the first charging cycle that increased to 96% after second cycle. The self-discharge test of the full-cell after charging to 2.7 V at C/5 current rate is showed a stable 2 V after 90 hours. The capacities of the developed batteries at lower currents are comparable to the metallic electrode-based devices, however, the capacities were observed to drop at higher currents. This makes the developed paper-based batteries more suitable for low current applications, such as, RFID tags, flexible electronics, bioassays, and displays. The capacities of the batteries at higher current can be improved by enhancing the conductivity of the fibers, which is identified as the future work. Furthermore, fabrication of an all solid state battery using solid electrolyte is also identified as the future work of this project.