Novel materials can be derived from cellulose biomass including highly crystalline nanofibrils (CNF) or nanowhiskers/crystals (CNC). Cellulose nanofibrils were first isolated from wood possessing transparency, biocompatibility, and excellent mechanical properties. These outstanding properties make nanofibrillated cellulose a good candidate in various advanced materials for biomaterials and electronic devices. Carbon materials including carbon black, graphite, graphene and their derivatives with zero-dimension, one-dimension, and three-dimension structures exhibit exceptional physical properties, such as high electron mobility, quantum Hall effects, and the excellent mechanical performance. Recently, nanocellulose challenges graphene as the new prodigy. One of the great challenges of nanocellulose is large-scale production, because, as with graphene, its limited production could make it unfeasible for use in certain technological applications. However, cellulose is found in large quantities in nature and, therefore, the challenge faced by researchers resides in synthesizing cellulose to obtain nanocellulose on a large scale. In this report, we conduct the combination of nanocellulose (nanofibrils or nanocrystals) and carbon materials (carbon black and graphite/grapheme oxide, grapheme) with different nanostructures to promotes high mechanical strength along with excellent toughness, high electrical conductivity and sensitive resistivity-response through innovative structuring methods to achieve synergetic properties that cannot be achieved in previously reported nanocellulose-based polymer nanocomposites. The functional composites based on nanocellulose and carbon materials can be fabricated by adjusting the morphology and structure to open the new field of nanocomposites.