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Lithium-ion batteries using flexible paper-based current collectors have been developed. These current collectors were fabricated from wood microfibers that were coated with carbon nanotubes (CNT) through an electrostatic layer-by-layer nanoassembly process. The carbon nanotube mass loading of the presented (CNT-microfiber paper) current collectors is 10.1 μg/cm2. The capacities of the batteries made with the current collectors are 150 mAh/g for lithium cobalt oxide (LCO) half-cell, 158 mAh/g for lithium titanium oxide (LTO) half-cell, and 126 mAh/g for LTO/LCO full-cell. The fabrication approach of the CNT-microfiber paper current collectors, the assembly of the batteries, and the experimental results are presented and discussed.