Cellulose is one of the most abundant organic materials on earth, and cellulose paper is ubiquitous in our daily life. Re-engineering cellulose fibers at the nanoscale will allow this renewable material to be applied to advanced energy storage systems and optoelectronic devices. In this article, we examine the recent development of nanofibrillated cellulose and discuss how the integration of other nanomaterials leads to a wide range of applications. The unique properties of nanofibrillated cellulose enable multi-scale structuring of the functional composites, which can be tailored to develop new concepts of energy and electronic devices. Tapping into the nanostructured materials offered by nature can offer many opportunities that will take nanotechnology research to a new level.