Nanopaper has attracted considerable interest in the fields of films and paper research. However, the challenge of integrating the many advantages of nanopaper still remains. Herein, we developed a facile strategy to fabricate multifunctional nanocomposite paper (NGCP) composed of wood-derived nanofibrillated cellulose (NFC) and graphene as building blocks. NFC suspension was consisted of long and entangled NFCs (10–30 nm in width) and their aggregates. Before NGCP formation, NFC was chemically modified with a silane coupling agent to ensure that it could interact strongly with graphene in NGCP. The resulting NGCP samples were flexible and could be bent repeatedly without any structural damage. Within the NGCP samples, the high aspect ratio of NFC made a major contribution to its high mechanical strength, whereas the sheet-like graphene endowed the NGCP with electrical resistance and electrochemical activity. The mechanical strength of the NGCP samples decreased as their graphene content increased. However, the electrical resistance and electrochemical activity of the NGCP samples both rose with increasing content of graphene. The NGCPs still kept advantageous mechanical properties even at high temperatures around 300°C because of the high thermal stability of NFCs and their strong entangled web-like structures. In view of its sustainable building blocks and multifunctional characteristics, the NGCP developed in this work is promising as low-cost and high-performance nanopaper