TEMPO oxidized cellulose nanofibrils (TOCNF) were used as binder material to prepare bendable Li4Ti5O12 (LTO) electrodes. Carbon fiber (CF) layers were integrated as current collectors to enhance the mechanical properties and to increase the specific energy of the electrodes. These electrodes combined with CF current collectors (LTO/CF) show good electrochemical properties and are flexible, sustainable, mechanical and chemical stable, lightweight and produced by a water-based easy filtration process. An increase of the active material weight (LTO) from around 19% to 71% of the electrode and current collector combined weight is demonstrated with CF compared with a copper current collector. Additionally, preparation of the current collector material is non-expensive, quick and easy compared to that of carbon nanotube or graphene. To test the flexible battery application, 4000 times repeated bending was carried out on both the LTO electrodes and the LTO/CF electrodes. This had no significant effect on the morphology, mechanical and electrochemical properties of neither the LTO nor the LTO/CF electrodes. Addition of the CF layer improves the mechanical properties and specific capacity of the LTO-electrode. A thicker LTO electrode with only 2wt% TOCNF is demonstrated which is promising for thicker electrodes with high energy density. A full cell was assembled with the LTO/CF as negative electrode and LiFePO4 (LFP)/CF as positive, which exhibited a stable cycling performance and good energy density.