A new spray coating water-based process is here proposed for the rapid and reliable large-scale production of self-standing Li-ion battery electrodes using truly natural microfibrillated cellulose as binder. The graphite/carbon black microfibrillated cellulose slurry was spray coated on a wet paper substrate which, subsequently pressed and dried on a conventional pilot paper machine, led to the formation of a bilayered electrode with excellent mechanical properties, cycling performances vs Li metal comparable to those of anodes with standard composition, (i.e. Young Modulus of 2.5 GPa and specific capacity of 350 mAh g(-1), at 0.1 C) but a Coulombic efficiency (ca. 98% in the first 50 cycles) which needs to be improved to maintain good cycling performances in Li-ion systems. This work demonstrated that well-established industrial papermaking techniques and materials can be adapted to the elaboration of well-functioning electrodes thus paving the way for the transfer the Li-ion battery industrial area of high-throughput paper production technologies. (C) 2013 Elsevier B.V. All rights reserved.